ArticlePDF Available

Occurrence and fate of methane leakage from cut and buried abandoned gas wells in the Netherlands


Abstract and Figures

Methane leakage caused by well integrity failure was assessed at 28 abandoned gas wells and 1 oil well in the Netherlands, which have been plugged, cut and buried to below the ground surface (≥3 mbgl). At each location, methane concentrations were thoroughly scanned at the surface. A static chamber setup was used to measure methane flow rates from the surface as well as from 1 m deep holes drilled using a hand auger. An anomalously high flow rate from 1 m depth combined with isotopic confirmation of a thermogenic origin revealed ongoing leakage at 1 of the 29 wells (3.4%), that had gone undetected by surficial measurements. Gas fluxes at the other sites were due to shallow production of biogenic methane. Detailed investigation at the leaking well (MON-02), consisting of 28 flux measurements conducted in a 2 × 2 m grid from holes drilled to 1 and 2 m depth, showed that flux magnitude was spatially heterogeneous and consistently larger at 2 m depth compared to 1 m. Isotopic evidence revealed oxidation accounted for roughly 25% of the decrease in flux towards the surface. The estimated total flux from the well (443 g CH4 hr−1) was calculated by extrapolation of the individual flow rate measurements at 2 m depth and should be considered an indicative value as the validity of the estimate using our approach requires confirmation by modelling and/or experimental studies. Together, our findings show that total methane emissions from leaking gas wells in the Netherlands are likely negligible compared to other sources of anthropogenic methane emissions (e.g. <1% of emissions from the Dutch energy sector). Furthermore, subsurface measurements greatly improve the likelihood of detecting leakage at buried abandoned wells and are therefore essential to accurately assess their greenhouse gas emissions and explosion hazards.
Content may be subject to copyright.
Occurrence and fate of methane leakage from cut and buried abandoned
gas wells in the Netherlands
Gilian Schout
, Jasper Grifoen
, S. Majid Hassanizadeh
, Guillaume Cardon de Lichtbuer
, Niels Hartog
Copernicus Institute of Sustainable Development, Utrecht University, 3584 CB Utrecht, the Netherlands
Earth Sciences Department, Utrecht University, 3584 CB Utrecht, the Netherlands
TNO Geological Survey of the Netherlands, 3584 CB Utrecht, the Netherlands
KWR Water Cycle Research Institute, 3433 PE Nieuwegein, the Netherlands
Monitoring for gas leakage at cut and
buried wells is complicated by several
Leakage was detected at 1 of 29 cut and
buried abandoned wells in the
Dispersion and oxidation in soils can
prevent detection by surcial measure-
Subsurface and isotopic measurements
needed to conrm and quantify meth-
ane leakage.
Cut and buried wells may constitute an
explosion hazard that needs to be
abstractarticle info
Article history:
Received 21 November 2018
Received in revised form 21 December 2018
Accepted 22 December 2018
Available online 24 December 2018
Editor: Frederic Coulon
Methane leakage caused by well integrity failure was assessed at 28 abandoned gas wells and 1 oil well in the
Netherlands, which have been plugged, cut and buried to below the ground surface (3 mbgl). At each location,
methane concentrations were thoroughly scanned at the surface. A static chamber setup was used to measure
methane ow rates from the surface as well as from 1 m deep holes drilled using a hand auger. An anomalously
high ow rate from 1 m depth combined with isotopic conrmation of a thermogenic origin revealed ongoing
leakage at 1 of the 29 wells (3.4%), that had gone undetected by surcial measurements. Gas uxes at the
other sites were due to shallow production of biogenic methane. Detailed investigation at the leaking well
(MON-02), consisting of 28 ux measurements conducted in a 2 × 2 m grid from holes drilled to 1 and 2 m
depth, showed that ux magnitude was spatially heterogeneous and consistently larger at 2 m depth compared
to 1 m. Isotopic evidence revealed oxidation accounted for roughly 25% of the decrease in ux towards the sur-
face. The estimated total ux from the well (443 g CH
) was calculated by extrapolation of the individual
ow rate measurements at 2 m depth and should be considered an indicativevalue as the validity of the estimate
using our approach requires conrmation by modelling and/or experimental studies. Together, our ndings
show that total methane emissions from leaking gas wells in the Netherlands are likely negligible compared to
other sources of anthropogenic methaneemissions (e.g. b1% of emissions from the Dutchenergy sector). Further-
more, subsurface measurements greatly improve the likelihood of detecting leakage at buried abandoned wells
and are therefore essential to accurately assess their greenhouse gas emissions and explosion hazards.
© 2019 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license (http://
Abandoned wells
Gas migration
Methane leakage
Well integrity
Static chamber measurements
Methane isotopes
Science of the Total Environment 659 (2019) 773782
Corresponding author at: Copernicus Institute of Sustainable Development, Utrecht University, 3584 CB Utrecht, the Netherlands.
E-mail address: (G. Schout).
0048-9697/© 2019 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license (
Contents lists available at ScienceDirect
Science of the Total Environment
journal homepage:
1. Introduction
Leakage of natural gas from oil and gas wells has been identied as
an environmental hazard for several decades (Dusseault et al., 2000;
Erno and Schmitz, 1996;Harrison, 1983). Not only does leakage from
oil and gas infrastructure appear to contribute signicantly to rising an-
thropogenic methane emissions and the associated greenhouse effect
(Miller et al., 2013;Rice et al., 2016), gas migrating into surrounding
geological strata adversely impacts groundwater in aquifers overlying
oil and gas reservoirs (Harrison, 1983;Kelly et al., 1985) and may
pose an explosion hazard (Chilingar and Endres, 2005). In recent
years, elevated levels of thermogenic methane in groundwater have
also been attributed to wellbore leakage from newer, unconventional
oil and gas wells (Darrah et al., 2014;Sherwood et al., 2016). Although
water containing methane is not considered a health hazard (Vidic
et al., 2013), the introduction of methane in a groundwater system
may result in changing redox conditions that in turn may lead to
water quality changes, such as increased sulde concentrations
(Gorody, 2012) or the mobilization of trace elements (Cahill et al.,
Recent conservative estimates suggest that at least four million on-
shore hydrocarbon wells have been drilled worldwide (Davies et al.,
2014). A well may leak if a conduit for uid migration exists from the
wellbore system to its surroundings, a situation that is referred to as
well integrity failure (King and King, 2013). Whether leakage to outside
the well occurs depends on the presence of a driving force. This explains
why buoyancy driven gas leakage is a more common observation than
leakage of liquids (Davies et al., 2014) and that the leakage risk appears
to be higher for gas wells than for oil wells (King and King, 2013). Other
attributes that play a role in determining leakage frequency are differ-
ences in well type (conventional versus unconventional), geographic lo-
cation, well age (Ingraffea et al., 2014), well depth (Watson and Bachu,
2009), and plugging status (Kang et al., 2016). Hence, observed failure
frequencies vary greatly between different basins, with reported values
rangingfrom1.9%toupto75%(Davies et al., 2014).
In addition to these well attributes, observed leakage frequencies
may also differ as a result of the monitoring method used. Detection
and quantication of gas leakage caused by well integrity failure is typ-
ically assessed at the wellhead using measurements of either sustained
casing pressure (SCP) (Brufatto et al., 2003;Lackey et al., 2017), surface
casing vent ow (SCVF) (Dusseault et al., 2014;Watson and Bachu,
2009) or visual observation of leaking gas bubbles. Furthermore, gas
leakage from oil and gas wells has also been assessed by measuring
the concentration and isotopic composition of dissolved gasses in
nearby groundwater wells (e.g. Osborn et al., 2011;Van Stempvoort
and Jaworski, 1995). However, the ability to detect leakage using
groundwater monitoring strongly depends on the distance between
the leakage point and the groundwater sampling location (Jackson
et al., 2013;Molofsky et al., 2011), the direction and velocity of ground-
water ow and the occurrence of microbial methane oxidation (Schout
et al., 2017;Van Stempvoort et al., 2005).
At abandoned oil and gas wells, monitoring options are often limited
by the lack of an intact wellhead. With the number of abandoned wells
growing rapidly (Dusseault et al., 2014), effective monitoring at these
wells will be crucial to identify and remedy methane leakage. At 88
abandoned oil and gas wells in Pennsylvania, USA, methane ow
could be measured by sealing a chamber over the remainder of aban-
doned wellbore systems protruding from the surface (Kang et al.,
2016). 90% of these wells were a positive source of methane, with gas
wells and unplugged wells emitting relatively large amounts of meth-
ane compared to oil wells and plugged wells. Besides plugging, some
oil and gas jurisdictions require that wells are cut to below the ground
surface and buried as the nal step in the abandonment process
(Davies et al., 2014). At such wells, detecting and quantifying a gas
leak at surface is complicated as it originates from an uncertain depth
below the surface.
Methaneow rates at 138 abandoned wells from fourUS states were
measured by Townsend-Small et al. (2016), including a subset of wells
that had been cut and buried. To measure leakage at these locations,
the surface above the well sites was rst scanned using mobile methane
detection instruments. When anomalous concentrations were detected,
methane uxes at the soil-atmosphere interface were measured using
ux chamber methodology and gas samples were collected for source
identication. Overall, the study showed that 42% of unplugged wells
compared to only 0.8% of plugged wells were a positive source of meth-
ane. Boothroyd et al. (2016) measured methane concentrations at the
soil-atmosphere interface above 102 plugged, cut and buried wells
that had been decommissioned according to best practice in the UK.
By comparing the measured concentrations to that at nearby control lo-
cations, ongoing leakage caused by well integrity failure was concluded
for 30% of these wells. However, the wells being the actual source of the
methane were not corroborated by gas sampling and isotopic analysis.
In addition, gas leaking from cut and buried wells has to migrate up-
ward through the vadose zone by diffusion and buoyancy, where it is
dispersed and may be partially oxidized before it can be detected at
the surface (Erno and Schmitz, 1996). Furthermore, preferential ow
paths may cause leaking gas to emerge offset with a considerable dis-
tance (N10 m) from a leaking wellbore (Forde et al., 2019).
Overall, both the environmental hazard of gas leakage at cut and
buried wells and the complexities of detecting and quantifying such
leakage have been understudied. So far, studies on methane leakage at
cut and buried abandoned gas wells did not account for the possibility
that signicant portions of leaking gas may be dispersed and oxidized
in the vadose zone, which could have led to an underestimation of the
actual occurrence and leakage rate. In the Netherlands, there are cur-
rently roughly 900 onshore oil and gas wells that have already been
abandoned (Table 1) and the effectivenessof past and present abandon-
ment procedures is largely unknown. Therefore, we selected 29
plugged, cut and buried wells for eld investigation into the occurrence
of gas leakage at these sites and to assess the importance of gas disper-
sion and oxidation in the vadose zone using static ux measurements
above holes drilled into the surface, in addition to methane ux mea-
surements and thorough concentration scanning at the surface. The
aims of the study were to evaluate (1) the potential methane leakage
from abandoned wells in the Netherlands and (2) the suitability of var-
ious methods for detecting and quantifying gas migration from aban-
doned wells that have been cut and buriedto below the ground surface.
2. Materials and methods
2.1. Oil and gas wells in the Netherlands
The Netherlands has a long history of oil and gas production, and has
been one of the major hydrocarbon producing countries in Europe. It
owes this mainly to the discovery of two large reservoirs: the
Schoonebeek oil eld in 1943 and the Groningen gas eld in 1959. In
combination with the discovery of numerous smaller elds, this has
led to the drilling of around 2500 hydrocarbon wells, of which N1700
onshore (Table 1). Gas production and drilling of new onshore wells
in the Netherlands has slowed down in recent decades, because of de-
pletion of reserves and induced seismicity in the Groningen area (van
Thienen-Visser and Breunese, 2015). Currently, around 85% of all
Table 1
Breakdown of oil and gas well status in the Netherlands (NLOG, 2018).
Active Closed-in Plugged/abandoned Other/ unknown Total
Onshore oil 29 64 706 27 826
Offshore oil 24 16 97 12 149
Onshore gas 439 212 191 64 906
Offshore gas 179 105 270 55 609
Total 671 397 1264 158 2490
774 G. Schout et al. / Science of the Total Environment 659 (2019) 773782
onshore oil wells and 20% of onshore gas wells have already been aban-
doned (Table 1). The Dutch mining law regulates abandonment proce-
dures of oil and gas wells. Besides prescribing detailed plugging
procedures (Van Der Kuip et al., 2011), it also mandates that onshore
wells are cut to at least three meter below the surface and buried
(6 m below the seaoor for offshore wells). While this lawdoes not pre-
scribe any post-abandonment monitoring, operators still carry respon-
sibility for the well according to Dutch civil law, should any deviation
from the abandonment regulations be uncovered later (i.e., if leakage
is detected) (Ministry of Economic Affairs, 2017).
Publicly available well integrity data from Dutch wells is limited. A
2011 assessment carried out by the State Supervision of Mines
(SodM) uncovered well barrier failure in 1 out of 26 production wells
and 3 out of 5 water injection wells for produced water (Vignes,
2011). However, well barrier failure does not necessarily equate to
well integrity failure (King and King, 2013), given that there are often
multiple barriers in place (e.g. several layers of casing and cement).
Hence, the risk that these wells pose collectively for both groundwater
quality and anthropogenic GHG emissions is unknown. Recently, ongo-
ing gas leakage was detected at one borehole where a catastrophic
blowout occurred while drilling this well in 1965, and as such it was
not abandoned according to protocol (Schout et al., 2017). Thus far,
this is the only known instance of methane leakage to groundwater in
the Netherlands.
2.2. Well selection
Hydrocarbon well locations and other meta-data were obtained
from the governmental Netherlands Oil and Gas Portal(NLOG, 2018).
Gas wells were prioritized over oil wells. No differentiation is made in
the database between wells that have only been plugged and those
that also have been cut and buried. Hence, a subset of such wells was
identied by visual inspection of satellite imagery, at which p oint acces-
sibility for eldwork was also estimated. For example, locations that
were built over already could not be included. Wells were selected
from the various gas reservoirs spread throughout the Netherlands. Fi-
nally, as most abandoned well locations are situated on private land, ac-
cessibility depended on obtaining permission from the landowner
during eldwork. Ultimately, measurements were carried out at 29 lo-
cations (Fig. 1) during June and July of 2017: 28 gas wells and 1 oil
well (RWK-14).
2.3. Surcial scanning
In the Netherlands, the locations of cut and buried hydrocarbon
wells are not visually marked at the ground surface. Hence, they had
to be located using GPS based on available coordinates. To decrease
the chance of missing methane emissions from a leaking well, methane
concentrations at the soil-atmosphere interface were rst scanned in a
circular area above the abandoned wells. A minimum radius of 15 m
was chosen, which was estimated to be much larger than the uncer-
tainty of the GPS and the given coordinates of the well. Scanning was
performed using a Gazomat TDL-500 Inspectra Laser, which measures
concentrations real-time with a resolution of 0.1 ppmv and was
checked for accuracy every day using a calibration gas cylinder
(50 ppmv). To scan each site thoroughly and in a repeatable manner,
the operator of the device was connected with a rope to a cylinder
(1 m circumference) placed at the coordinates of the well and had to
walk in circles around this cylinder while keeping the rope tight. The
resulting spiraling pattern (known as the involute of a circle,Fig. 2)
places the operator closer to the well every lap with a distance equal
to the circumference of the cylinder.
A rod with a suction cup was attached to the inlet of the device
(Fig. 2) that was held just above the soil surface during the scanning
and moved from side to side while walking slowly. Additionally, the
suction cup was placed directly on the soil at regular intervals and left
for 510 s, after which methane concentrations and GPS coordinates
were recorded. The locations of any deviating values were marked for
subsequent analysis with static chamber ux measurements. The dis-
tance along the spiral in between measurements was decreased to-
wards the well, such that the density of measurements was highest
near the well location. Scanning in this manner yielded an overall aver-
age of around 160 data points per well. Maps of the recorded values for
each well location are shown in Fig. S1.
2.4. Static chamber measurements
Static chamber measurements were carried out directly above the
buried remains of the well and, for 22 of the 29 well sites, a control
Fig. 1. Locations of the 29investigated abandoned wellstogether with theoil and gas elds
in the Netherlands (NLOG, 2018).
Fig. 2. Photo of the surcial scanning in action. Operator is attached to a wooden cylinder
placed on the estimated location of the buried well, as marked with a red dot. The black
line schematically shows the remaining path to be wa lked. (For interpr etation of the
references to color in this gure legend, the reader is referred to the web version of this
775G. Schout et al. / Science of the Total Environment 659 (2019) 773782
location. For consistency, controls were taken at the starting pointof the
surcial scanning, i.e., a minimum of 15 m away from the well. This dis-
tance was expected to be larger than the uncertainty range associated
with locating the well. However, the soil at this location would still be
similarly affected by the abandonment procedure of the well (pad),
local land use and soil conditions. Measurements wereadditionally con-
ducted at locations that had elevated methane concentrations during
the scanning.
A plexiglas cylindrical chamber (Fig. 3) with a height of 56 cm and a
radius of 11.5 cm was used (volume of 23.25 L). To limit gas exchange
with the atmosphere, the cylinder was placed on a plastic ring that
was pushed 10 cm into the ground. Methane concentrations in the cyl-
inder were recorded at regular intervals using the Gazomat TDL-500,
also used for the surcial scanning. Both the inlet and outlet of this de-
vice were connected to the chamber with exible tubing, such that
measured gas was returned to the chamber (Fig. 3). The pumping rate
of the device was 70 L hr
, which ensured mixing inside the cylinder.
After completion of the measurements at the soil surface, 1 m deep
open holes were drilled using a hand auger (5 cm diameter). Measure-
ments were then directly repeated above the newly drilled holes (with
the ring still in place).
The mass ow rate into the chamber was calculated using linear re-
gression on the concentration versus time data (Eq. 1).
where F is the CH
ow rate (mg hr
), dC/dt is the rate of change in
concentration in the chamber [mg cm
] and V the chamber
volume [cm
]. Similar to previous studies (Kang et al., 2016, 2014),
only linear ts with an R
value N0.8 were considered. R
values below
0.8 only occurred when the concentration in the chamber remained
close to the atmospheric methane concentration. Hence, the methane
ow at these locations was assumed to be zero. Measurements were
discontinued if no trend or change in concentrations inside the chamber
was observed after 5 min. While the measurement resolution was
0.1 ppmv, experience learned that measured concentrations sometimes
drifted slightly, going up and down within a bandwidth of around
0.5 ppmv. Assuming a temperature of 18 °C and a pressure of 1 atm,
the minimum mass ow that would result in a positive determination
within 5 min (ΔCH
0.5 ppmv) was 0.09 mg hr
. In some cases the
measurement period was extended to lower this detection limit
2.5. Analysis of gas samples for stable methane isotopes
Gas samples for isotopic analyses were collected upon completion of
the static chamber measurements by placing 1 L tedlar bags in a sealed
box attached directly to the static chamber.Vacuum was created in this
box using a foot pump, causing the sample bags to ll with gas from the
chamber. As measured uxes were generally higher at 1 m depth, it was
decided to collect samples after these measurements rather than those
at the surface. Samples were collected at additional locations if methane
leakage from the abandoned well was suspected. Analyses of the sam-
ples were carried out at the Institute for Atmospheric and Marine Re-
search (IMAU) of the Utrecht University. Methane was extracted as
described in Röckmann et al. (2016): methane carbon (δ
hydrogen (δ
) stable isotope ratios were determined in separate
measurements by Isotope RatioMass Spectrometry (IRMS) on a Thermo
Finnigan Delta plus XP. The sample mixing ratio and isotopic composi-
tion were determined by comparing the measurements to that of a
known reference air that was extracted in the same way.
2.6. Detailed characterization of methane leakage at the MON-02 site
Thermogenic methane was observed at well MON-02 following the
previously described procedures. This site was therefore characterized
in more detail. Well MON-02 produced from the Monstergas eld
(Fig. 1), a small gas accumulation in the West Netherlands Basin, and
was abandoned in the 1990s. The reservoir consists of a series of Triassic
layers known together as the Main Bundsandstein Subgroup, and is sit-
uated at a depth around 2800 to 3000 m. Starting at the coordinates of
the abandoned wellbore, static chamber measurements were carried
out in each cardinal direction with a 2 m spacing. Once a negligible
ux was identied at 1 m depth, measurements were continued in the
next direction. This procedure led to 14 measurement locations that
form a grid like pattern, with each measurement representing an area
of 2 by 2 m. In addition to the procedure described in Section 2.4,static
chamber measurements were also conducted at 2 m depth, slightly
above the groundwater table at this location (2.2 mbgl). This was
done by extending the already drilled holes to 2 m once the 1 m deep
measurements were completed. Furthermore, PVC tubes with the
same length and diameter (5 cm) as the drilled holes were placed inside
the holes and connected directly to the chamber so that ow into the
chamber could only occur from the bottom of the tube. A sandy soil pro-
le was encountered throughout the site. Samples for isotopic analysis
were collected at the end of seven measurements of a single transect:
three at 1 m depth and four at 2 m depth.
In total, 28 static ux measurements were carried out (Table S.2).
Regression was performed over a linear part of the data (R
0.8) of
at minimum 50 s in order to calculate the ow rates. To estimate the
total leakage ux from the well the methane ow rates were converted
to a measured mass ux (Eq. 2):
where J
is the measured CH
ux [mg cm
is the surcial
area of the opening of the tube [cm
]. Due to the lack of a porous me-
dium inside the tube, the diffusive ux towards the chamber was en-
hanced compared to the initial, undisturbed soil condition. To account
for this, measurements were scaled by the ratio of the diffusion
Fig. 3. Schematic representation of the static chamber measurements carried out above
plugged, cut and buried wells. Chamber dimensions were 56 cm height, 11.5 cm radius,
23.25 L volume. Static chamber measurements were rst carried before drilling the 1 m
hole on which additional static chamber measurements were conducted. Figure not to
776 G. Schout et al. / Science of the Total Environment 659 (2019) 773782
coefcient of methanein sandy soil to that in air,yielding an approxima-
tion of the undisturbed ux:
where J
is the estimated undisturbed methane ux [mg cm
and D
the effective diffusion coefcient in sandy soil and the diffu-
sion coefcient in air, respectively [cm
]. A D
of 726 cm
assumed according to the method of Fuller et al. (1966) for CH
at 18
°C and 1015 mbar. The effective diffusion coefcient in sandy soil was
calculated as follows (e.g. Scanlon et al., 2002):
Deff ¼ϕτSgDað4Þ
where ϕis the porosity [], S
is the saturation of the gas phase []and
τthe tortuosity factor (determined according to Penman, 1940a, 1940b.
A porosity of 0.3 and soil gas saturation of 0.9 were assumed. Finally, the
total leakage ux from the well was calculated by means of a nearest
neighbor interpolation, at 1 and 2 m depth separately: rst, the esti-
mated undisturbed ux for each measurement location was extrapo-
lated to the 2 × 2 m square area surrounding it and then all data
points were summed.
3. Results
3.1. Surcial scanning
Surcial scanning of methane concentrations at the soil-atmosphere
interface was carried out fully at 19 and partly at 5 of the 29 selected
well sites (Fig. S1). At 10 locations obstructions such as canals or
dense undergrowth either partially or fully limited the required mobil-
ity (see for example Fig. 4B). During the course of most measurements,
observed concentrations tended to drift around the atmospheric meth-
ane concentration (~1.8 ppmv) between roughly 1.1 and 2.5 ppmv.
Thus, observed patterns of both increasing and decreasing concentra-
tions could not be related to locally enhancedmethane emissions or up-
take by the soil as long as the concentration changes remained within
this bandwidth (e.g. Fig. 4AandFig. 4B). Isolated locations with concen-
trations N2.5 ppmv were observed at6 well sites (Fig. S1). In most cases,
these observations were temporary concentration spikes and could not
be reproduced on subsequent measurements. However, these locations
were marked for laterinvestigation using the static chambersetup. Only
while scanning well site NKK-01elevated methane concentrations up to
several hundred ppmv were observed that also sustained over a longer
time period (Fig. 4C).
3.2. Static chamber measurements at surface and 1 m depth
The static chamber measurements carried out at the soil surface di-
rectly above the 29 buried wells revealed only a single location with a
positive methane ow rate: AKM-07 (Fig. 5, Table S.1). In contrast,
ow rateswere negative at thesurface above fourwells, and no measur-
able methane ow was recorded above the remaining wells. The sur-
cial static chamber measurements also revealed two positive and one
negative ow rate at the control locations; ow could not be detected
at the remaining control locations. Negative ow rates are interpreted
as methane uptake from the soil caused by methane oxidation in the va-
dose zone. At 1 m depth, positive methane ow rates were observed
more frequently than at the surface while negative ow rates were
only observed at two control locations. Overall, 15 of 29 well locations
and 10 of 22 control locations had a positive methane ow rate at 1 m
depth (Fig. 5). With the exception of well NKK-01, measurements car-
ried out at locations that were marked because of concentration outliers
observed during the surcial scanning did not yield appreciably higher
ow rates. Hence, these measurements were not considered for further
Methane ow rates at 1 m depth were larger above the buried wells
than at their respective control for 6 locations. Conversely, control mea-
surements were larger at 8 other locations (Fig. 5). The remaining 8 lo-
cations where control measurements were conducted had undetectable
ow rates both above the buried wells and at the control locations. As
can be seen in Fig. 5, the variability in ow rate between the well and
control locations was such that the difference between them could not
be relied upon to attribute measured ow rates above the buried
wells to well integrity failure. A clear positive outlier was, however, ob-
served at well MON-02 with a ow rate of 1418 mg hr
at 1 m depth.
This is more than two orders of magnitude higher than the nexthighest
ow rate measurement in the entire study. Furthermore, this high ow
rate contrasted with the negative ow rate measured at 1 m depth at
the control location, the undetectable ow rates at the surface and the
lack of elevated concentrations recorded during the surcial scanning
(Fig. 4A).
3.3. Analysis methane stable isotopes
Only the sample collected after the ux measurement at 1 m depth
above well MON-02, where the highest single ux measurement was
observed, had a clear thermogenic origin (δ
C-CH4 = 26.6and
δD-CH4 = 149.7,Fig. 6). This is convincing evidence that leakage
of natural gas caused by well integrity failure was occurring. Samples
from other locations with high ow rates had isotopic compositions
Fig. 4. Three examples of the results obtained during surcial scanning of methane concentrations: A) MON-02, B) WYK-30, where only half the scanning spiral could be executed and
C) NKK-01, where several concentration outliers were identied that were marked for static chamber ux measurements.
777G. Schout et al. / Science of the Total Environment 659 (2019) 773782
indicative of a biogenic origin, with a δ
b50and a δD-CH
225, regardless of whether the uxes above the well or at the con-
trol location had given higher uxes. A biogenic gas source was also con-
rmed at well NKK-01, the only location where high methane
concentrations where recorded during the surcial scanning that also
resulted in positive ow rate measurements at the surface. The bacterial
methane is likely related to the presence of organic-rich formations,
abundant in the shallow subsurface of the Netherlands. Many oil and
gas elds in the Netherlands are found in the coastal provinces, where
Holocene peat and clay deposits are also present (Wong et al., 2007).
Methane emissions from these deposits are well known (Van Den Pol-
Van Dasselaar et al., 1999). Samples from locations with intermediate
ow rates showed isotopic compositions that can be explained by
mixing of biogenic and atmospheric methane, while sites with zero or
low ow rates showed an atmospheric origin with δ
and δD-
values of around 47and 93, respectively (Fig. 6).
3.4. Detailed characterization of methane leakage at the MON-02 site
The detailed characterization carried out at well MON-02 showed
that the estimated undisturbed methane uxes were signicantly
higher at 2 m depth than at 1 m depth (Fig. 7). At the location directly
overlying the coordinates of the abandoned wellbore (A1), the esti-
mated undisturbed ux at 1 m depth was 9.4 g m
compared to
19.6 g m
at 2 m depth. While the maximum ux at 1 m depth
was located at the coordinates of the well, the maximum ux at 2 m
depth was located almost 3 m to the south (B2) and was 4.5 times larger
than the maximum ux at 1 m depth: 40.4 g CH
able lateral spreading is observed with uxes N2gm
up to 4.5 m distance from the well coordinates at 1 m depth and up to
6 m at 2 m depth. If subsurface methane concentrations had solely
been the result of diffusion from a buried point source through a homo-
geneous, sandy porous medium (as encountered at the site), spreading
would have occurred in semi-spherical manner in all directions equally.
However, this is not thecase, as illustrated by the fact that the uxes just
2 m northeast of the coordinates of the well (O1) were zero at both 1
and 2 m depth. Nearest neighbor interpolation of the data yielded a
total leakage ux estimate of 111 g hr
at 1 m depth and 443 g hr
at 2 m depth. At atmospheric pressure and a temperature of 18 °C,
this is equal to a volumetric ux of 4.0 and 15.8 m
Furthermore, it suggests that a reduction in ux of 74% had occurred
from 2 to 1 m depth.
Isotopic compositions of the 7 collected samples at MON-02 varied
signicantly (Fig. 8). The isotopic composition of methane from the
Monster gas reservoir is known from a publicly available analysis of a
gas sample collected from nearby gas well MON-03 (NLOG, 2018). The
sample collected at the location with the lowest ux (A4-2 m) lies
close to the mixing line of gas from the reservoir and atmospheric meth-
ane. The samples that are isotopically most similar to that of the reser-
voir are three samples collected at 2 m depth at the locations with the
highest ux measurements (A1-2 m, A2-2 m and A3-2 m). Relative to
these three samples, two of the samples from 1 m depth (A1-1 m and
A3-1 m) are enriched in both their carbon and hydrogen isotopic com-
position. This is indicative of the occurrence of aerobic microbial meth-
ane oxidation as the isotopic fractionation factors observed for aerobic
methane oxidation in Dutch and German soils (α
C = 1.008 and αD
=1.0039,Bergamaschi et al., 1998) qualitatively match the shift from
the samples collected at 2 m depth to those at 1 m depth (Fig. 8). Fol-
lowing the methods described in Whiticar (1999), the observed shift
can be related to a residual methane fraction of 75%. In other words,
methane oxidation can account for up to 25% of the reduction in meth-
ane ux as observed from 2 to 1 m depth.
The isotopic composition of sample A2-1 m, which is isotopically de-
pleted compared to the reservoir gas, represents an outlier that cannot
be explained by leakage of gas from the Monster gas reservoir. Possibly
the leaking gas here does not originate from the reservoir, but rather
from an intermediate formation. The most likely candidate is the Hol-
land Greensand Member, a known gas-bearing formation in the
Netherlands located here at a depth of 1420 to 1481 m. The isotopic
composition of this formation is known from two samples taken from
a nearby small gas eld (Fig. 8) and matches that of the sample taken
at A2-1 m relatively well.
Fig. 5. Methane ow rates at thesurface (A) and at 1 m depth (B) as determined by static
chamber ux measurements. Locations are shown that have at minimum one non-zero
measurement (22 out of 29 locations). Grey area is below the detection limit (BDL),
locations where no control measurements were carried out are labelled with ´NC´.
Fig. 6. Carbon and hydrogen isotopic composition of methane in samples collected after
completion of static chamber measurements at 1 m depth. Grey dots show isotopic
composition of samples taken from onshore Dutch gas reservoirs (NLOG, 2018). Isotopic
composition of northern-hemisphere atmospheric methane based on Rice et al. (2016).
778 G. Schout et al. / Science of the Total Environment 659 (2019) 773782
4. Discussion
4.1. Detecting gas leakage from cut and buried abandoned wells
As shown by the results of our study, the occurrence of gas leakage at
cut and buried abandoned wells is more easily missed when relying on
surface measurements only, as compared with abandoned wells that
still have existing wellhead infrastructure protruding to the surface. Be-
sides additional uncertainties on the exact location of the buried well,
particularly in the absence of surface markers (as is the case in the
Netherlands), leaking methane may become dispersed and oxidized as
it migrates from the leakage point towards the surface, not necessarily
at the well coordinates due to preferential ow paths. When a lea k orig-
inates below the groundwater table, upwardly migrating methane can
be additionally attenuated by dissolution into groundwater (Cahill
et al., 2017). Obviously, when gas leakages result from well integrity
failure at greater depth and the gas migrates along the outside of the
casing these processes would equally affect methane transport to sur-
face (Dusseault and Jackson, 2014), regardless of whether a well is
abandoned, cut and buried, or still protruding to the surface. A combina-
tion of these processes caused leakage from a gas well in Colorado, USA,
to be undetectable by surcial ux measurements and soil gas probes
installed to 60 cm depth, while methane concentrationsin the underly-
ing groundwater were above air-saturation levels (McMahon et al.,
2018). Subsurface (vadose zone) measurements using dedicated soil
gas wells have previously been employed in soils surrounding oil and
gas wells that were notcut and buried by (Lyman et al., 2017). However,
while this allows for continued and precise monitoring of soil gas con-
centrations, our method is lesscostly and time consuming and therefore
enables relatively quick screening at multiple locations.
Methane leakage from a cut and buried wellbore may also be
masked by mixing with naturally occurring biogenic methane. Such
emissions can be highly spatially variable as a result of soil heterogene-
ities and preferentialpathways (Hendrikset al., 2010). This is illustrated
in our study by the detection of hotspots of elevated methane concen-
trations during the surcial scanning at several locations above one
well (NKK-02; Fig. 4C), but where isotopic analysis revealed a shallow
biogenic origin. Furthermore, local variabilities in biogenic methane
uxes also explain the lack of correlation between the magnitude of
the uxes measured at surface and 1 m depth as well as their controls
(Fig. 5). Given these conditions, isotopic conrmation of methane origin
is critically important in preventing false negatives or positives in the
detection of subsurface gas leakage from a well. At the one well in this
study for which gas leakage was conrmed, both the surcial scanning
and the surface static chamber measurements did not yield any notice-
able indication of leakage (MON-02; Fig. 4A, Fig. 5). This emphasizes the
importance of subsurface measurements of methane ow rates or con-
centrations, above the level from where leaks could be occurring, as dis-
persion and oxidation will have had less impact on the methane ux
Fig. 7. Results of the detailed investigation at MON-02: values signify the estimated undisturbed uxes at 1 m depth (left) and 2 m depth (right), contours depict the underground
spreading of leaked methane but are speculative. Grey inlay shows the label for each position, the red line indicates the locations at which samples were collected for isotopic analysis.
(For interpretation of the references to color in this gure legend, the reader is referred to the web version of this article.)
Fig. 8. Isotopic composition and estimated undisturbed ux of seven samples collected as
part of the detailed investigation at MON-02 (sampling positions indicated by red line in
gure inlay). Two thermogenic end members are shown: Monster reservoir gas (MON-
03) and gas from the intermediate Holland Greensand Member (HGM; NLOG, 2018).
Red dashed line shows the estimated effect of aerobic methane oxidation, red labels the
estimated residual methane fraction. Calculation based on isotopic fractionation factors
found in soils above Dutch landlls (ΔD/ΔC = 4.8, Bergamasc hi et al., 1998). (F or
interpretation of the references to color in this gure legend, the reader is referred to
the web version of this article.)
779G. Schout et al. / Science of the Total Environment 659 (2019) 773782
than at the surface. Also, for conditions of high background biogenic
methane production, the dilution and mixing of the isotopic signature
of the leaking gas would be smaller.
Although oxidation and dispersion decrease the detectability of
methane leakage, isotopic analysis can, in addition to determination of
origin, aid in determining the relative importance of these two pro-
cesses in the total attenuation of the subsurface methane ux from a
cut and buried well. As shown by the enrichment of the methane isoto-
pic composition (Fig. 8) concurrent with the decrease in ux between 2
and 1 m below ground surface for the gas leakage occurring at well
MON-02 (Fig. 7), aerobic methane oxidation accounted for roughly
25% of this decrease. Hence, around 75% of the decrease in methane
ux towards the surface was attributable to dispersion for that well
site. Negative uxes, resulting from the net oxidation of methane were
indeed observed at several of the investigated locations, including at
the control location of well MON-02 (Fig. 5). Furthermore, the wide-
spread oxidation of subsurface methane uxes (whether biogenic or
thermogenic) is also suggested by the consistently larger uxes mea-
sured at 1 m depth than those measured at the surface for the other lo-
cations investigated (Fig. 5). The extent to which dispersion and
oxidation affect the methane ux from subsurface well leakage will
however strongly vary between different well locations, depending on
the depth of the leakage point, as well as a range of local physical (e.g.
water content) and biochemical (e.g. redox conditions, microbialpopu-
lation) conditions and the heterogeneities therein.
4.2. Estimation of the total methane leakage ux from cut and buried aban-
doned wells
At abandoned wells thatare not cut and buried,sealing the wellhead
off from the atmosphere allows for accurate measurements of the total
leakage ux (assuming there is no gas migration outside the casing). At
cut and buried wells however, quantication of the total ux is more
complex as each measured ux represents an unknown portion of the
total ux. Furthermore, while necessary for the detailed characteriza-
tion of leakage at MON-02, carrying out ux chamber measurements
from holes drilled into the soil introduces additional uncertainty by
disturbing soil properties and the initial methane concentration distri-
bution in the vadose zone. The three most notable sources of uncer-
tainty include rst that we had to compensate for the lack of a porous
medium in the tube installed into the drilled holes by scaling the mea-
sured ux with the ratio of the effective diffusion coefcient of methane
in soil over the diffusion coefcient of methane in pure air. This requires
knowledge of the porosity, tortuosity and gas saturation of the porous
medium, which we did not determine in the eld and hence had to be
approximated. Second, the measurements for the detailed investigation
did not yield strictly linearly increasing concentration versus time data.
Hence, regression analysis had to becarried out on the linear part of the
data for that particular ux measurement. The non-linear behavior was
likely caused by a combination of factors, includingthe alteration of soil
properties due the drilling, non-vertical and possibly some advective in-
ow of methane into the tubes, and disruption of the initial methane
concentration prole in the soil. Third, interpolation of the measure-
ments at 2 m depth assumes that methane uxes are strictly vertical
whereas in reality there is an important lateral component (as also
shown by the results of our study). Further, the interpolation assumes
that the ux is more or less spatially distributed and not dominated by
uxes through preferential ow paths. We believe this to be generally
valid heregiven the sandy conditions and the lack of concentration out-
liers observed during the surcial scanning.
Given the number of sources of uncertainty and the assumptions re-
quired under these non-ideal subsurface leakage conditions, our esti-
mation of the ux at 2 m depth (443 g CH
or 15.8 m
should be considered an indicative value only. Also, vadose zone pro-
cesses have been shown to lead to considerable temporal variation of
methane uxes measured by static ux chambers (Forde et al., 2018),
and our measurements thus only represent a snapshot of the total leak-
age ux at one moment in time. Longer term monitoring would be rec-
ommended to better constrain the average ux from a leaking well.
Future modelling and/or experimental studies may help to determine
the validity of the approach taken for the estimation of total leakage
ux. In comparison to leakage ux estimates in other studies, our total
ux estimate at two-meter depth is larger than any of the uxes identi-
ed at plugged wells by both Townsend-Small et al. (2016) and Kang
et al. (2016).However,theux estimate is in the same order of magni-
tude as the maximum uxes they observed at unplugged wells. In com-
parison, surface casing vent ow uxes appear to be much larger on
average: uxes larger than 10 m
were observed at 32% of
11,394 conventional wells with reported leakage issues in Alberta and
British Columbia, Canada (Nowamooz et al., 2015). Therefore, our indic-
ative total ux estimate does not seem unrealistic.
4.3. Observed well leakage frequency in context
This study revealed that methane leakage caused by integrity failure
had occurred at 1 out of 28 cut and buried abandoned gas wells (3.6%).
While this value is at the low end of the large range reported for well in-
tegrity failure in the review by Davies et al. (2014), it is considerably
higher than the 0.060.15% found by Sherwood et al. (2016) in Colo-
rado,USA.However,theirndings were based on water chemistry anal-
yses, which is a more indirect measurement and may therefore have
contributed to a relatively low leakage frequency. The observed well
leakage frequency is larger than that found by Townsend-Small et al.,
2016 (0.8%) for plugged and abandoned oil and gas wells, part of
which had also cut and buried, but lower than both the 30% reported
by Boothroyd et al. (2016) for plugged, cut and buried wells in the UK
and the 62% reported by Kang et al., 2016 for plugged wells that had
not been cutand buried. These differences are likely caused by a combi-
nation of factors such as the local geology, well type, well construction,
well abandonment procedures (King and King, 2013) and the type of
monitoring method employed. Here, the amount of wells studies likely
plays a role, too. More studies are needed in order to obtain proper in-
sight in the statistics of well integrity failure for the Netherlands as
well as globally.
4.4. Environmental impact of abandoned gas wells in the Netherlands
Given the limited amount of wells studied, extrapolation of the re-
sults can only be done tentatively. Using binomial statistics, the lower
and upper probability that could have still resulted in 1 positive detec-
tion within one standard deviation were calculated to convert our nd-
ings to a range. This yields a well integrity failure rate for cut and buried
gas wells in the Netherlands of between 1.4% to 9.0%,which is equal to a
range of between 3 and 17 leaking wells when extrapolating to all cur-
rently abandoned gas wells (n= 191) and between 12 and 81 leaking
wells when extrapolating to the total amount of onshore gas wells (n
= 906). Assuming each well leaks with the estimated ux at 2 m
depth at well MON-02, this gives a rough national estimate of between
10 and 66 ton CH
emitted for the abandoned gas wells, or be-
tween 48 and 315 ton CH
for all gas wells. This is equal to between
0.14 and 0.95% of the total amount of CH
estimated to have been emit-
ted by the Dutch energy sector in 2015, and 0.0050.035% of the total
anthropogenic CH
emissions in the country (Environmental Data
Compendium, 2017). In other terms, the maximum estimated value is
equal to the methane produced by roughly 500 Dutch milk cows
(~133 kg CH
;Velthof et al., 2016). Concluding, it is improb-
able that the methane leaking from these wells contributes signicantly
to current anthropogenic GHG gas emissions in the Netherlands.
In the case of cut and buried wells, part of the leaking methane is
converted to CO
as a result of aerobic oxidation. Hence, combining
methane concentration measurements with CO
measurements would
be required to fully assess GHG emissions. Given that methane has a
780 G. Schout et al. / Science of the Total Environment 659 (2019) 773782
global warming potential 24 times that of CO
(Myhre et al., 2013), CO
emitted in this manner is likely insignicant for our study area. Notably,
leakage from cut and buried oil and gaswells does have to be considered
in the context of explosion hazards. This is illustrated by the MON-02
case reported in this study, where the intended construction of several
new houses was upheld to repair the leaking abandoned well and en-
sure the safety of the new buildings.
5. Conclusions
Methane leakage fromcut and buried abandoned oil and gas wells is
an understudied environmental hazard, and the detection and quanti-
cation of leakage at such wells is complex. To assess environmental im-
pact and effective monitoring methods, 28 cut and buried gas wells and
1 oil well were investigated in the Netherlands. Leakagewas observed at
1 gas well (MON-02), constituting the rst observation of well integrity
failure at a properly decommissioned gas well in the country. Neither
the surcial methane concentration scanning nor the static ux mea-
surements carried out at the surface proved capable of detecting the
leaking gas. However, static ux measurements above 1 m deep holes
drilled into the soil were an effective method. In general, measured
ow rates were consistently larger at depth than at the surface. Control
measurements showed that naturally occurring biogenic methane
uxes were spatially highly variable. Therefore, the origin of measured
uxes could not be determined based on ux magnitude alone, and
analyses of methane stable isotopes were required to distinguish be-
tween a biogenic or thermogenic origin.
A detailed characterization at the leaking well, consisting of static
chamber measurements in conducted in a 2 × 2 grid from holes drilled
to 1 and 2 m depth, showed that measured ow rates diminished rap-
idly towards the surface. Enrichment of the isotopic composition con-
current with this decrease conrmed that besides dispersion, aerobic
methane oxidation accounted for roughly 25% of this decrease.
Converting the ow rate measurements in the vadose zone to a total
ux estimate is not trivial, as each measurement represents only a
small portion of the total ux and the drilling of the holes required for
the measurements disturbs the soil properties. Nevertheless, an indica-
tive value wascomputed by converting each measurement at 2 m depth
to estimates of the undisturbedux and then interpolating using
nearest neighbor interpolation. This approach yields a value of
443 g CH
emitted from the well. Extrapolating this number to
all - abandoned or not - gas wells (n= 906) in the Netherlands and tak-
ing an uncertainty range of 1.4 to 9.0% for the well integrity failure rate
yields a rst estimate of 48315 ton CH
. This is negligible com-
pared to the yearly methane emissions from the energy sector
(0.140.95%) and overall anthropogenic methane emissions
(0.0050.035%) in the Netherlands.
Taken together, these ndings support the need for subsurface mea-
surements when trying to detect and quantify methane leakage from
cut and buried gas wells, and have important implications for past and
future studies aimed at detecting methane leakage at such wells. How-
ever, more research is required to assess whether point measurements
of vadose zone methane uxes can be reliable converted to estimates of
the total leakage ux from a cut and buried well. In spite of considerable
uncertainty, our results show that leakages from gas wells are unlikely
to contribute signicantly to GHG emissions in the Netherlands. How-
ever, the potential explosion hazard caused by methane leakage from
cut and buried abandoned wells needs to be taken into account when
planning construction projects.
Supplementary data to this article can be found online at https://doi.
We thank KWR Watercycle Research Institute for providing guid-
ance on eld methods and eld materials, Carina van der Veen for
carryingout the analyses of our samplesat the IMAU lab, and Hans Oonk
for making available his portable methane analyzer for our study. This
work is part of the research program Shale Gas and Waterwith project
number 859.14.001, which is nanced by the Netherlands Organization
for Scientic Research (NWO).
Bergamaschi, P., Lubina, C., Königstedt, R., Fischer, H., Veltkamp, A.C., Zwaagstra, O., 1998.
Stable isotope signatures (d13C, dD) of methane f rom European landll sites.
J. Geophys. Res. 103, 82518265.
Boothroyd, I.M., Almond, S., Qassim, S.M., Worrall, F., Davies, R.J., 2016. Fugitive emissions
of methane from abandoned, decommissioned oil and gas wells. Sci. Total Environ.
547, 461469.
Brufatto, C., Cochran Aberdeen, J., Lee Conn David Power, S., Zaki Abd Alla El-Zeghaty, S.,
Fraboulet, B., Grifn, T., James Trevor Munk, S., Justus Santa Cruz, F., Joseph Levine,
B.R., Montgomery, C., Murphy, D., Pfeiffer Houston, J., Tiraputra Pornpoch, T., Rishmani
Abu Dhabi, L., 2003. From mud to cementbuilding gas Wells. Oilf. Rev. 6276.
Cahill, A.G., Steelman, C.M., Forde, O., Kuloyo, O., Emil Ruff, S., Mayer, B., Ulrich Mayer, K.,
Strous, M., Cathryn Ryan, M., Cherry, J.A., Parker, B.L., 2017. Mobility and persistence
of methane in groundwater in a controlled-r elease eld experiment. Nat. Geosci.
Chilingar, G.V., Endres, B., 2005. Environmental hazards posed by the Los Angeles Basin
urban oilelds: an historical perspective of lessons learned. Environ. Geol. https://
Darrah, T.H., Vengosh, A., Jackson, R.B., Warner,N.R., Poreda, R.J., 2014. Noble gases iden-
tify the mechanisms of fugitive gas contamination in drinking-water wells overlying
the Marcellusand Barnett Shales. Proc.Natl. Acad. Sci. 111, 1407614081. https://doi.
Davies, R.J., Almond, S., Ward, R.S., Jackson, R.B., Adams, C., Worrall, F., Herringshaw, L.G.,
Gluyas, J.G., Whitehead, M.A., 2014. Oiland gas wells and their integrity: implications
for shale and unconventional resource exploitation. Mar. Pet. Geol. 56, 239254.
Dusseault, M., Jackson, R., 2014. Seepage pathway assessment for natural gas to shallow
groundwater during well stimulation, in production, and after abandonment. Envi-
ron. Geosci. 21, 107126.
Dusseault, M.B., Gray, M.N., Nawrocki,P.A., 2000. Why oilwellsleak: cement behaviorand
long-term consequences. SPE International Oil and Gas Conference and Exhibition.
64733, p. 8.
Dusseault, M.B., Jackson, R.E., MacDonald, D., 2014. Towards a road map formitigating the
rates and occurrences of long-term wellbore leakage. Georma 169.
Environmental Data Compendium, 2017. Greenhouse gas emissions the Netherlands,
19902016. [WWW Document].
house-gas-emissions, Accesse d date: 7 J uly 2018.
Erno, B., Schmitz, R., 1996. Measurements of soil gas migration around oil and gas wells in
the Lloydminster area. J. Can. Pet. Technol. 35, 3746.
Forde, O.N., Mayer, K.U., Cahill, A.G., Mayer, B., Cherry, J.A., Parker, B.L., 2018. Vadose zone gas
migration and surface efuxes after a controlled natural gas release into an unconned
shallow aquifer. Vadose Zo. J. 17, 0.
Forde, O.N., Mayer, K.U., Hunkeler,D., 2019. Identication, spatial extent and distribution
of fugitive gas migrat ion on the well pad scale. Sci. Total Environ. 652, 356366.
Fuller, E.N., Schettler, P.D., Giddings, J.C.,1966. A new method for prediction of binary gas-
phase diffusion coefcients.Ind.Eng.Chem.58,1827.
Gorody, A.W., 2012. Factors affecting the variability of stray gas concentration and com-
position in groundwater. Environ . Geosci. 19, 1731.
Harrison, S.S., 1983. Evaluating system for ground-water contamination hazards due to
gas-well drilling on the glaciated Appalachian plateau. Groundwater 21, 689700.
Hendriks, D.M.D., van Huissteden, J., Dolman, A.J., 2010. Multi-technique assessment of
spatial and temporal variability of methane uxes in a peat mead ow. Agric. For.
Ingraffea, A.R., Wells, M.T., Santoro, R.L., Shonkoff, S.B.C., 2014. Assessment and risk analysis
of casing and cement impairment in oil and gas wells in Pennsylvania, 20002012. Proc.
Natl. Acad. Sci. 111, 1095510960.
Jackson, R.B., Vengosh, A., Darrah, T.H., Warner, N.R., Down, A., Poreda, R.J., Osborn, S.G.,
Zhao, K., Karr, J.D., 2013. Increa sed stray gas abundance in a subset of drinking
water wells near Mar cellus shale gas extraction. Proc . Natl. Acad. Sci. 11 0,
Kang, M., Kanno, C.M., Reid, M.C., Zhang, X., Mauzerall, D.L., Celia, M.A., Chen, Y., Onstott,
T.C., 2014. Direct measurements of methane emissions from abandoned oil and gas
wells in Pennsylvania. Proc. Natl. Acad. Sci. U. S. A. 111, 1817318177. https://doi.
Kang, M., Christian, S., Celia, M.A., Mauzerall, D.L., Bill, M., Miller, A.R., Chen, Y., Conrad,
M.E., Darrah, T.H., Jac kson, R.B., 2016. Identication and charact erization of high
methane-emitting abandoned oil and gas wells. Proc. Natl. Acad. Sci. 113,
Kelly, W.R., Matisoff, G., Fisher, J.B., 1985. The effects of a gas well blow out on groundwater
chemistry. Environ. Geol. Water Sci. 7, 205213.
King, G.E., King, D.E., 2013. Environmental risk arising from well-construction failure
differences between barrier and wellfailure, and estimates of failure frequency across
common welltypes, locations, and well age. SPE Prod.Oper. 28, 323344. https://doi.
781G. Schout et al. / Science of the Total Environment 659 (2019) 773782
Lackey, G., Rajaram, H., Sherwood, O.A., Burke, T.L., Ryan, J.N., 2017. Surface casing pres-
sure as an indicator of well integrity loss and stray gas migration in the Wattenberg
Field, Colorado. Environ. Sci. Technol. 51, 35673574.
Lyman, S.N., Watkins, C., Jones, C.P., Manseld, M.L., McKinley, M., Kenney, D., Evans, J.,
2017. Hydrocarbon and carbon dioxide uxesfrom natural gas wellpad soils and sur-
rounding soils in eastern Utah. Environ. Sci. Technol. 51, 1162511633. https://doi.
McMahon,P.B., Thomas, J.C.,Crawford, J.T.,Dornblaser, M.M.,Hunt, A.G., 2018. Methane in
groundwater from a leaking gas well, Piceance Basin, Colorado, USA. Sci. Total Envi-
ron. 634, 791801.
Miller, S.M., Wof sy, S.C., Michalak, A.M., Kort, E.A., Andrews, A.E., Biraud, S.C.,
Dlugokencky, E.J., Eluszkiewicz, J., Fischer, M.L., Janssens-Maenhout, G., Miller, B.R.,
Miller, J.B., Montzka, S.A., Nehrkorn, T., Sweeney, C., 2013. Anthropogenic emissions
of methane in the United States. Proc. Natl. Acad. Sci. 110, 2001820022. https://
Ministry of Economic Affairs, 20 17. Beantwoor ding Kamervrag en over lekkages bij
AkzoNobel in Twente (2017Z07676).
Molofsky, L.J., Connor, J.A., Farhat, S.K., Wylie, A.S., Wagner, T., 2011. Methane in Pennsyl-
vania water wells unrelated to Marcellus shale fracturing. Oil Gas J. (December 5),
Myhre, G., Shindell, D., Bréon, F.-M., Collins, W., Fuglestvedt, J., Huang, J., Koch, D.,
Lamarque, J.-F. , Lee, D., Mendoza, B., Nakajima, T., Robock, A., Ste phens, G.,
Takemura, T., Zhang, H., 2013. Anthropogenic and Na tural Radiative Forcing. In:
Stocker, T.F., Qin, D., Plattner, G.-K., Tignor, M., Allen, S.K., Boschung, J., Nauels, A.,
Xia, Y., Bex, V., Midgley, P.M. (Eds.), Climate Change 2013: The Physical S cience
Basis. Contribution of Working Group I to the Fifth Assessment Report of the Inter-
governmental Panel on Climate Change. Cambridge University Press, Cambridge,
United Kingdom and New York, NY, USA.
NLOG, 2018. Netherl ands oil and gas portal deep borehole data. [WWW Document]., Accessed date: 6 July 2018.
Nowamooz, A., Lemieux, J.M., Molson, J., Therrien, R., 2015. Numerical investigation of
methane and formation uid leakage along the casing of a decommissioned shale
gas well. Water R esour. Res. 51, 45924622.
Osborn, S.G., Vengosh, A., Warner, N.R., Jackson, R.B., 2011. Methane contamination of
drinking water accompanying gas-well drilling and hydraulic fracturing. Proc. Natl.
Acad. Sci. 108, E665E666.
Penman, H.L., 1940a. Gas andvapour movements in the soil: II. The diffusion of carbon di-
oxide through porous solids. J. Agric. Sci. 30, 570. https://
Penman, H.L., 1940b. Gas and vapour movements in the soil: I. the diffusion of vapours
through porous solids. J. Agric. Sci. 30, 437.
Rice, A.L., Butenhoff, C.L., Teama, D.G., Röger, F.H., Khalil, M.A.K., Rasmussen, R.A., 2016.
Atmospheric methane isotopic record favors fossil sources at in 1980s and 1990s
with recent increase. Proc. Natl. Acad. Sci. 113 , 1079110796.
Röckmann, T., Eyer, S., Van Der Veen, C., Popa, M.E., Tuzson, B., Monteil, G., Houweling, S.,
Harris, E., Brunner, D., Fischer, H., Zazzeri, G., Lowry, D., Nisbet, E.G., Brand, W.A.,
Necki, J.M., Emme negger, L., Mohn, J., 2016. In s itu observations of the isotopic
composition of me thane at the Cabau w tall tower site. Atmos. Chem. Phys. 16,
Scanlon, B.R., Nicot, J.P., Massmann, J.W., 2002. Soil gas movement in unsaturated sys-
tems. In: Warrick, A.W. (Ed.), Soil Physics Companion. Taylor & Francis Group, Boca
Ration, pp. 297341
Schout, G., Hartog, N., Hassanizadeh, S.M., Grifoen, J., 2017. Impact of an historic under-
ground gas well blowout on the current methane chemistry in a shallow groundwa-
ter system. Proc. Natl. Acad. Sci. 115 (201711472).
Sherwood, O.A., Rogers, J.D., Lackey, G., Burke, T.L., Osborn, S.G., Ryan, J.N., 2016. Ground-
water methane in relation to oil and gas development and shallow coal seams in the
Denver-Julesburg Basin of Colorado. Proc. Natl. Acad. Sci. 113 (201523267). https://
Townsend-Small, A., Ferrara, T.W., Lyon, D.R., Fries, A.E., Lamb, B.K., 2016. Emissions of
coalbed and natural gas methane from abandoned oil and gas wells in the United
States. Geophys. Res. Lett. 43, 22832290.
Van den Pol-van Dasselaar, A., Van Beusichem, M.L., Oenema, O., 1999. Methane emis-
sions from wet grasslands on peat soil in a nature preserve. Biogeochemistry 44,
Van Der Kuip, M.D.C., Benedictus, T., Wildgust, N., Aiken, T., 2011. High-level integrity as-
sessment ofabandoned wells. Energy Procedia, 53205326
Van Stempvoort, D., Jaworski, E., 1995. Migration of Methane into Groundwater from
Leaking Production Wells Near Lloyd Minster. Calgary, Canada.
Van Stempvoort, D., Maathuis, H., Jaworski, E., Mayer, B., Rich, K., 2005. Oxidation of fugi-
tive methanein ground water linked to bacterial sulfate reduction. Ground Water 43,
van Thienen-Visser, K.,Breunese, J.N., 2015.Induced seismicity of theGroningen gas eld:
history and recent developments. Lead. Edge 34, 664671.
tle34060 664.1.
Velthof, G.L., Van Bruggen, C., Groenestein, C.M., Huijsmans, J.F.M., Luesink, H.H., Van Der
Sluis, S.M., Van der Kolk, J.W.H., Voshaar, S.V.O., Vonk, J., Van Schijndel, M.W., 2016.
Referentieram ing van emissies naar lucht uit de landbouw tot 2030.;
Achtergronddocument bij de Nationale Energieverkenning 2015, met emissies van
ammoniak, methaan, lachgas, stikstofoxide en jnstof uit de landbouw tot 2030.
Vidic, R.D., Brantley, S.L., Vandenbossche, J.M., Yoxtheimer, D., Abad, J.D., 2013. Impact of
shale gas development on regional water quality. Science 340, 1235009. https://doi.
Vignes, B.,2011. Contribution to Well Integrityand Increased Focus on Well Barriers From
a Lifecycle Aspect. University of Stavanger.
Watson, T.L., Bachu, S., 2009. Evaluation of the potential for gas and CO2 leakage along
wellbores. SPE Drill. Complet. 24, 115126.
Whiticar, M.J., 1999. Carbonand hydrogen isotope systematics of bacterial formation and
oxidation of methane. Chem. Geol. 161, 291314. http s://
Wong, T.E.,Batjes, D.A.J., de Jager, J., 2007. Geology of the Netherlands. Royal Netherlands
Academy of Arts and Sciences, Amsterdam.
782 G. Schout et al. / Science of the Total Environment 659 (2019) 773782
... We reviewed 27 studies measuring CH 4 emissions from OGWs at the wellhead scale. We excluded studies measuring CH 4 emissions from offshore wells (Gorchov Negron et al., 2020) and studies not differentiating between emissions from multiple point 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 A c c e p t e d M a n u s c r i p t Bishop, 2013;Ho et al., 2016;Alboiu and Walker, 2019;Kang et al., , 2021Abboud, Watson and Ryan, 2020;Lavoie et al., 2022 Leakage Gasda, Bachu and Celia, 2004;Miller et al., 2013;Davies et al., 2014;Kang et al., 2014;Pétron et al., 2014;Warneke et al., 2014;Nathan et al., 2015;Zavala-Araiza et al., 2015Allen, 2016;Boothroyd et al., 2016;Omara et al., 2016;Townsend-Small et al., 2016;Atherton et al., 2017;Emran, Tannant and Najjaran, 2017;Johnson et al., 2017;Lavoie et al., 2017;Moortgat, Schwartz and Darrah, 2018;Pekney et al., 2018;Cahill et al., 2019;Fox et al., 2019;Hoschouer and Townsend-Small, 2019;Johnson, Heltzel and Oliver, 2019;Pandey et al., 2019;Riddick et al., 2019;Schout et al., 2019;Whiticar, 2019;Deighton et al., 2020;Ingraffea et al., 2020;Lebel et al., 2020;Wisen et al., 2020;MacKay et al., 2021;Singh et al., 2021;Williams et al., 2021;El Hachem and Kang, A c c e p t e d M a n u s c r i p t ...
... Therefore, CH 4 emission rates at abandoned wells are more frequently measured at the individual source level with methods requiring site access (Kang et al., 2014;Forde et al., 2019;Riddick et al., 2019;Williams et al., 2021;Bowman et al., 2022;El Hachem and Kang, 2022); only four studies used mobile surveys to quantify emissions from abandoned wells (Johnson and Heltzel, 2016;Atherton et al., 2017;Lebel et al., 2020;Vogt et al., 2022). The most common approaches to measure CH 4 emissions from abandoned OGWs are based on chambers or enclosures (Kang et al., 2014), atmospheric modeling (Riddick et al., 2019;Lebel et al., 2020), Hi-Flow samplers (Pekney et al., 2018), and soil gas sampling (Boothroyd et al., 2016;Schout et al., 2019). Aerial surveys using helicopters and drones have primarily been used to find abandoned wells and not to measure emission rates . ...
Full-text available
Oil and gas wells (OGWs) with integrity failures can be a conduit for methane and contaminant leakage to groundwater aquifers, surface water bodies and the atmosphere. Recent reviews have addressed OGW leakage but focused on specific types of wells (conventional/unconventional) or specific geographic regions. Here, we conduct a literature review and focus on factors and policies affecting leakage of active and abandoned OGWs, studies quantifying OGW methane emissions, and leakage repair and emission reduction options. Of the 38 factors reviewed here in published literature, studies find that 15 (39%) factors, including geographic location, well deviation, casing quality and plugging status consistently affect OGW leakage. For 15 (39%) factors, including surface casing depth, well elevation and land cover, one or two studies show that they do not affect OGW leakage. For the remaining eight (21%) factors, including well age, studies show conflicting results. Although increased frequency of well monitoring and repair can lead to reduced OGW leakage, several studies indicate that monitoring and repair requirements are not always enforced. Moreover, we find that while 27 studies quantify OGW methane emissions to the atmosphere at the oil and gas wellhead scale, there still are major gaps in the geographical distribution of the collected data, especially for abandoned and orphaned wells. Although studies measuring abandoned wells may include measurements from orphaned wells, these measurements are not separated by well status (orphaned/abandoned), which is important for policy makers aiming to plug thousands of orphaned wells. To repair OGW leakage, we find that most studies focus on well cement and casing repair, and other studies focus on improving the cement mixture to avoid the need for repairs. Alternatives to cement and casing repair for methane emission reductions, such as soil methane oxidation to reduce leakage from OGWs may be effective, but their widespread applicability requires further study. Overall, our review of factors affecting OGW leakage can be used to guide OGW leakage monitoring and repair policies to target wells with high leakage potential, thereby reducing climate and environmental impacts.
... Moreover, a focus on methane emissions may lead to an emphasis on high methane emitters, which may lead to limited evaluation of the full suite of environmental risks. For surface water and groundwater contamination potential, methane emission rates measured at the surface are not likely to be a good proxy [54,55]. In addition, there is potential for plugging to reduce methane emissions but enhance groundwater contamination [56]. ...
Full-text available
Hundreds of thousands of documented and undocumented orphaned oil and gas wells exist in the United States (U.S.). These wells have the potential to contaminate water supplies, degrade ecosystems, and emit methane and other air pollutants. Thus, orphaned wells present risks to climate stability and to environmental and human health, which can be reduced by plugging. To quantify environmental risks and opportunities of well plugging at the national level, we analyze data on 81 857 documented orphaned wells across the U.S. We find that > 4.6 million people live within 1 km of a documented orphaned well. 35% of the documented orphaned wells are located within 1 km of a domestic groundwater well, yet only 8% of the wells have groundwater quality data within a 1 km radius. Methane emissions from the documented orphaned wells represent approximately 3%–6% of total U.S. methane emissions from abandoned oil and gas wells, but this estimate is based on measurements at < 0.03% of U.S. abandoned wells. 91% of the documented orphaned wells overlie formations favorable for geologic storage of carbon dioxide and hydrogen, meaning that orphaned well plugging can reduce leakage risks from future storage projects. Finally, we estimate plugging costs for documented orphaned wells to exceed the $4.7 billion federal funding by 30%–80%, emphasizing the importance of prioritizing federal spending on wells with large remediation benefits. Overall, environmental monitoring data are not extensive enough to quantify risks, especially those related to air and water quality and human health. Plugging orphaned wells can provide opportunities for geologic storage of carbon dioxide and hydrogen and geothermal energy development, thereby facilitating efforts to transition to net-zero energy systems. Our analysis on environmental risks and opportunities of orphaned wells provides a framework that can be used to manage the millions of documented and undocumented orphaned wells in the U.S. and abroad.
... Several studies from the past decade have shown that Oil and Gas (O&G) wells may continue to emit methane after production has ceased (Boothroyd et al., 2016;El Page 1 of 15 AUTHOR SUBMITTED MANUSCRIPT -ERC-101055. R2 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 A c c e p t e d M a n u s c r i p t Hachem and Kang, 2022;Kang et al., 2016;Kang et al., 2014;Lebel et al., 2020;Pekney et al., 2018;Riddick et al., 2019;Saint-Vincent et al., 2020;Saint-Vincent et al., 2021;Schout et al., 2019;Townsend-Small et al., 2016;Townsend-Small and Hoschouer, 2021;Williams et al., 2021;Williams et al., 2019). Methane (CH 4 ) is a powerful greenhouse gas (GHG) with a global warming potential 29.8 (± 11) times that of carbon dioxide (CO 2 ) over a period of 100 years, and controlling fugitive CH 4 emissions is an effective near-term pathway to mitigate the effects of climate change (Forster et al., 2021;Lecocq et al., 2021). ...
Full-text available
In 2018, the U.S. EPA Greenhouse Gas Inventory (GHGI) began including methane emissions from abandoned oil and gas (AOG) wells and estimated that they may constitute up to 4% of total methane emissions from the oil and gas sector. Several studies have shown that these emissions vary by location which introduces regionally dependent uncertainty into inventory estimates. In Wyoming, there are over 1000 wells identified as "orphaned" indicating that they are both abandoned and unplugged, approximately 80% of which are coalbed methane (CBM) wells. In this pilot study, 3-hour measurements of ten orphaned CBM wells were taken to support the characterization of AOG well emission rates in the Powder River Basin (PRB) in Wyoming. The mean methane emission rate measured at these wells was 653 mg CH4/hr with the majority of these wells emitting in the 100-1000 mg CH4/hr range. The highest emitting well in the study was measured at 4.53 g CH4/hr. Compared to the GHGI AOG wells emission factor of 10.04 g CH4/hr, these findings suggest that AOG wells emission rate in the PRB are overestimated by national inventory methods. Finally, the addition of AOG well emissions data from this study doubles the number of sampled AOG wells in Wyoming and triples the number of sampled CBM wells in the U.S..
... It is also reported that about 25% of wells in the Gulf of Mexico have sustained casing pressure leading to about a 50 million dollar per year expenditure on remedial works to fix cement failures (Cavanagh et al., 2007). Elsewhere in the Netherlands (Schout et al., 2019), established that 1 out of 29 plugged wells is leaking some formation fluid into the environment. Other researchers such as (Kyle Ferrar, 2019;Watson and Bachu, 2009;Vielstädte et al., 2015;Chukwuemeka et al., 2017) have also identified additional leakages and studied the potentials for CO 2 and methane leakage from abandoned wells (Kaiser, 2017). ...
... Numerous studies have confirmed that microseepage of CH 4 on the surface (soil, subsoil, and shallow aquifers) originates from deep gas-oil reservoirs [16][17][18]. There has been a preliminary understanding of CH 4 emissions from shale gas extraction [19][20][21][22], production/abandoned oil and gas wells, and their effects on the environment in recent years [23][24][25]. However, little research focused on the migration and release mechanisms of hydrocarbons [26,27]. ...
Full-text available
Methane (CH4) microseepage from petroleum basins is a significant contributor to the atmospheric CH4 budget. However, research about CH4 migration and release mechanism is still very limited. This work seeks to theorize and verify the migration and release mechanism of CH4 microseepage via field measurement and physical simulation, which, to the best of our knowledge, has not been reported in literature. Fluxes of CH4 microseepage from Dawanqi oilfield were measured, and three manifestations of release were observed, namely, continuous, flat, and episodic. Based on field observations, bench-scale physical simulation of CH4 migration through geological features of the oilfield was further conducted for 290 days. The results show that CH4 migration is mainly driven by buoyancy and diffusion. In continuous release, CH4 migration is mainly driven by buoyancy. In flat release, CH4 migration is dominated by diffusion. At low pressure, CH4 migrates upward slowly. As buoyancy increases, CH4 eventually break through the capillary pressure of the pore throat, causing spikes in CH4 concentrations in the layers above and reproducing episodic release observed during field measurement. Via field observation and verification by physical simulation, this work theorizes the migration mechanism of CH4 microseepage and its correlation with release types observed and confirms that counterbalance of buoyancy force and capillary pressure plays a critical role in episodic release of CH4 from oilfield. The findings of this study shed light on the migration mechanism and release manifestations of CH4 microseepage under different geological conditions and improve accuracy of estimating the flux of CH4 microseepage into atmosphere.
Conference Paper
Portland cement is commonly used in wells to provide zonal isolation in the annulus. A damaged cement sheath can expose the casing to corrosive fluids and open a leakage pathway to shallow freshwater aquifers and atmosphere. The leakage can manifest itself as sustained casing pressure (SCP) or lead to gas accumulation in shallower formations. The impact of pressure and temperature variation on cement stress has been widely studied in the literature. However, the hydration reactions of cement are not usually included in the mechanical models. This leads to incorrect assumptions about the initial state of stress in cement immediately after curing. In this work, we have developed a 3D well integrity model that incorporates the cement hydration process. The model is verified using laboratory experiments on cement stress evolution. The model calculates the water consumption during the hydration reactions to predict the pore pressure change in cement. The evolution of cement's mechanical properties with the hydration degree is captured using a homogenization model. A case study is designed to represent a typical low-enthalpy geothermal well in the Netherlands, using well designs and inputs from publicly available data. The cement stresses are tracked over the life of the well, to understand the magnitude of the stress cycles and to assess the potential long-term damage to the cement sheath. The results show that the pore pressure drop due to cement hydration causes an increase in shear stress in the cement sheath. The pore pressure drop during hydration can debond the cement from the formation. The level of destressing in cement is a function of cement properties, formation stiffness, and the depth of the top of cement. When placed against softer formations, the stress drop in cement is more muted leading to a better seal. During the temperature cycles, the shear stress in cement changes in a cyclical manner. Depending on the magnitude of the stress cycles, damage can be accumulated in the cement sheath. The stress evolution in cement can also vary depending on the presence of external water (formation permeability). The modelling technique presented in this work provides a robust methodology to estimate the magnitude of cyclical stresses in the cement sheath. This is a critical input to design cement recipes that can withstand load cycles throughout the lifetime of the well. The results of this work indicate the need to assess the integrity of cement at various depths and against various formations. It may not be possible to guarantee the seal efficiency against all formations, however risk analysis can be conducted using the presented model to assess the seal integrity of critical locations in the well profile.
Environmental risk assessment is generally based on atmospheric conditions for the modelling of chemical fate after entering the environment. However, during hydraulic fracturing, chemicals may be released deep underground. This study therefore focuses on the effects of high pressure and high temperature conditions on chemicals in flowback water to determine whether current environmental fate models need to be adapted in the context of downhole activities. Crushed shale and flowback water were mixed and exposed to different temperature (25-100 °C) and pressure (1-450 bar) conditions to investigate the effects they have on chemical fate. Samples were analysed using LC-HRMS based non-target screening. The results show that both high temperature and pressure conditions can impact the chemical fate of hydraulic fracturing related chemicals by increasing or decreasing concentrations via processes of transformation, sorption, degradation and/or dissolution. Furthermore, the degree and direction of change is chemical specific. The change is lower or equal to a factor of five, but for a few individual compounds the degree of change can exceed this factor of five. This suggests that environmental fate models based on surface conditions may be used for an approximation of chemical fate under downhole conditions by applying an additional factor of five to account for these uncertainties. More accurate insight into chemical fate under downhole conditions may be gained by studying a fluid of known chemical composition and an increased variability in temperature and pressure conditions including concentration, salinity and pH as variables.
Full-text available
Core Ideas Subsurface gas migration results in localized surficial CH 4 releases. Surficial CH 4 emissions show pronounced temporal variations. Methane concentrations in soil gas exceed lower explosive limits at low leakage rates. Increasing CO 2 effluxes and stable C isotope signatures indicate vadose zone CH 4 oxidation. Instantaneous surficial effluxes do not indicate the magnitude of subsurface gas leakage rates. Shale gas development has led to concerns regarding fugitive CH 4 migration in the subsurface and emissions to the atmosphere. However, few studies have characterized CH 4 migration mechanisms and fate related to fugitive gas releases from oil or gas wells. This paper presents results from vadose zone gas and surface efflux monitoring during a natural gas release experiment at Canadian Forces Base Borden, Alliston, Ontario, Canada. Over 72 d, 51 m ³ of natural gas (>93% CH 4 ) was injected into a shallow, unconfined sand aquifer at depths of 4.5 and 9 m. Methane and CO 2 effluxes in combination with soil gas concentrations and stable C isotopic signatures were used to quantify the spatiotemporal migration and fate of injected gas. Preferential gas migration pathways led to vadose zone hot spots, with CH 4 concentrations exceeding the lower explosive limit (5% v/v). From these hot spots, episodic surface CH 4 effluxes (temporally exceeding 2500 μmol m ⁻² s ⁻¹ [3465 g m ⁻² d ⁻¹ ]) occurred during active injection. Higher injection rates led to increased average CH 4 effluxes and greater lateral migration, as evidenced by a growing emission area approaching 25 m ² for the highest injection rate. Reactive transport modeling showed that high CH 4 fluxes resulted in advection‐dominated migration and limited CH 4 oxidation, whereas lower CH 4 effluxes were diffusion dominated with substantial CH 4 oxidation. These results and our interpretations allowed us to develop a conceptual model of fugitive CH 4 migration from the vadose zone to the ground surface.
Technical Report
Full-text available
Ter onderbouwing van de referentieraming van de uitstoot van broeikasgassen en luchtverontreinigende stoffen voor de Nationale Energie Verkenning 2015 (NEV 2015) zijn berekeningen uitgevoerd met het model NEMA (National Emission Model for Agriculture) van de emissies van ammoniak (NH3), stikstofoxide (NOx), fijnstof (PM10 en PM2,5), lachgas (N2O) en methaan (CH4) uit de landbouw voor de periode 2015-2030. De raming is uitgevoerd voor één referentiescenario, waarbij twee beleidsvarianten (vastgesteld en voorgenomen beleid op peildatum 1 april 2015) zijn onderscheiden. Daarnaast zijn gevoeligheidsanalyses uitgevoerd met betrekking tot dieraantallen, mestproductie, bemestingsgraad, aandeel emissiearme stallen en ureumkunstmestgebruik. De geraamde stikstofexcretie door de veestapel in Nederland neemt toe van 473 naar 490 miljoen kg in de periode 2013-2020 en neemt daarna geleidelijk af tot 481 miljoen kg in 2030. De fosfaatexcretie neemt in deze periode af van 166 naar 162 miljoen kg. De ammoniakemissie vanuit de landbouw neemt in de raming bij vastgesteld en voorgenomen beleid af met 15,8 miljoen kg in periode 2013-2030; van 112,3 miljoen kg NH3 in 2013 tot 96,5 miljoen kg in 2030. De methaanemissie neemt toe met 6%, de lachgasemissie neemt af met 3% en de stikstofoxide-emissie neemt toe met 1% in deze periode. De emissie van fijnstof kleiner dan 10 μm (PM10) neemt met 15% af en die van fijnstof kleiner dan 2,5 μm (PM2,5) neemt met 8% af.
Full-text available
Blowouts present a small but genuine risk when drilling into the deep subsurface and can have an immediate and significant impact on the surrounding environment. Nevertheless, studies that document their long-term impact are scarce. In 1965, a catastrophic underground blowout occurred during the drilling of a gas well in The Netherlands, which led to the uncontrolled release of large amounts of natural gas from the reservoir to the surface. In this study, the remaining impact on methane chemistry in the overlying aquifers was investigated. Methane concentrations higher than 10 mg/L (n = 12) were all found to have δ13C-CH4 values larger than -30‰, typical of a thermogenic origin. Both δ13C-CH4 and δD-CH4 correspond to the isotopic composition of the gas reservoir. Based on analysis of local groundwater flow conditions, this methane is not a remnant but most likely the result of ongoing leakage from the reservoir as a result of the blowout. Progressive enrichment of both δ13C-CH4 and δD-CH4 is observed with increasing distance and decreasing methane concentrations. The calculated isotopic fractionation factors of ε C = 3 and ε D = 54 suggest anaerobic methane oxidation is partly responsible for the observed decrease in concentrations. Elevated dissolved iron and manganese concentrations at the fringe of the methane plume show that oxidation is primarily mediated by the reduction of iron and manganese oxides. Combined, the data reveal the long-term impact that underground gas well blowouts may have on groundwater chemistry, as well as the important role of anaerobic oxidation in controlling the fate of dissolved methane.
Full-text available
Expansion of shale gas extraction has fuelled global concern about the potential impact of fugitive methane on groundwater and climate. Although methane leakage from wells is well documented, the consequences on groundwater remain sparsely studied and are thought by some to be minor. Here we present the results of a 72-day methane gas injection experiment into a shallow, flat-lying sand aquifer. In our experiment, although a significant fraction of methane vented to the atmosphere, an equal portion remained in the groundwater. We find that methane migration in the aquifer was governed by subtle grain-scale bedding that impeded buoyant free-phase gas flow and led to episodic releases of free-phase gas. The result was lateral migration of gas beyond that expected by groundwater advection alone. Methane persisted in the groundwater zone despite active growth of methanotrophic bacteria, although much of the methane that vented into the vadose zone was oxidized. Our findings demonstrate that even small-volume releases of methane gas can cause extensive and persistent free phase and solute plumes emanating from leaks that are detectable only by contaminant hydrogeology monitoring at high resolution.
Full-text available
The risk of environmental contamination by oil and gas wells depends strongly on the frequency with which they lose integrity. Wells with compromised integrity typically exhibit pressure in their outermost annulus (surface casing pressure, SfCP) due to gas accumulation. SfCP is an easily measured but poorly documented gauge of well integrity. Here, we analyze SfCP data from the Colorado Oil and Gas Conservation Commission database to evaluate the frequency of well integrity loss in the Wattenberg Test Zone (WTZ), within the Wattenberg Field, Colorado. Deviated and horizontal wells were found to exhibit SfCP more frequently than vertical wells. We propose a physically meaningful well-specific critical SfCP criterion, which indicates the potential for a well to induce stray gas migration. We show that 270 of 3,923 wells tested for SfCP in the WTZ exceeded critical SfCP. Critical SfCP is strongly controlled by the depth of the surface casing. Newer horizontal wells, drilled during the unconventional drilling boom, exhibited critical SfCP less frequently than other wells because they were predominantly constructed with deeper surface casings. Thus, they pose a lower risk for inducing stray gas migration than legacy vertical or deviated wells with surface casings shorter than modern standards.
Full-text available
Significance Millions of abandoned oil and gas wells exist across the United States and around the world. Our study analyzes historical and new field datasets to quantify the number of abandoned wells in Pennsylvania, individual and cumulative methane emissions, and the attributes that help explain these emissions. We show that ( i ) methane emissions from abandoned wells persist over multiple years and likely decades, ( ii ) high emitters appear to be unplugged gas wells and plugged/vented gas wells, as required in coal areas, and ( iii ) the number of abandoned wells may be as high as 750,000 in Pennsylvania alone. Knowing the attributes of high emitters will lead to cost-effective mitigation strategies that target high methane-emitting wells.
Global methane (CH4) emissions are becoming increasingly important due to the contribution of CH4 to global warming. Leaking oil and gas wells can lead to subsurface CH4 gas migration (GM), which can cause both aquifer contamination and atmospheric emissions. Despite the need to identify and quantify GM at oil and gas well pads, effective and reliable monitoring techniques are lacking. In this field study, we used CH4 and carbon dioxide (CO2) efflux measurements together with soil gas stable carbon isotopic signatures to identify the occurrence and to characterize the spatio-temporal migration of fugitive gas across 17 selected well pads in Northeastern British Columbia, Canada. At 13 of these sites, operators had previously reported the occurrence of GM; however, subsequent inspections based on visual, olfactory or auditory evidence only identified GM at two of these sites. Using the soil gas efflux method, evidence for GM was found at 15 of the 17 well pads with CH4 and CO2 effluxes ranging from 0.017 to 180 μmol m⁻² s⁻¹(0.024 to 250 g CH4 m⁻² d⁻¹) and 0.50 to 32 μmol m⁻² s⁻¹ (1.9 to 122 g CO2 m⁻² d⁻¹), respectively. Stable carbon isotopic composition was assessed at 10 of the 17 well pads with 9 well pads showing evidence of GM. The isotopic values indicated that CH4 in soil gas was from the same origin as CH4 in the surface casing vent flow gas. There was no correlation between CH4 effluxes and the distance from the well head; an equal portion of elevated effluxes were detected >10 m from the well head as were detected <5 m from the well head. In addition, CH4 effluxes varied temporally with values changing by up to an order of magnitude over 2 h. Although the study was carried out in Northeastern British Columbia, the results are applicable on a global scale, suggesting that inspections mostly based on visual evidence (e.g. bubbling at the well head) are not reliable for the identification of GM and, that infrequent survey measurements at predefined locations close to the well head may overestimate, underestimate or even miss CH4 effluxes. Repetitive and relatively densely spaced gas efflux measurements using a dynamic closed chamber method proved to be a useful tool for detecting GM.
We measured fluxes of methane, non-methane hydrocarbons, and carbon dioxide from natural gas well pad soils and from nearby undisturbed soils in eastern Utah. Methane fluxes varied from less than zero to more than 38 g m-2 h-1. Fluxes from well pad soils were almost always greater than from undisturbed soils. Fluxes were greater from locations with higher concentrations of total combustible gas in soil and were inversely correlated with distance from well heads. Several lines of evidence show that the majority of emission fluxes (about 70%) were primarily due to subsurface sources of raw gas that migrated to the atmosphere, with the remainder likely caused primarily by re-emission of spilled liquid hydrocarbons. Total hydrocarbon fluxes during summer were only 39 (16, 97)% as high as during winter, likely because soil bacteria consumed the majority of hydrocarbons during summer months. We estimate that natural gas well pad soils account for 4.6×10-4 (1.6×10-4, 1.6×10-3)% of total emissions of hydrocarbons from the oil and gas industry in Utah's Uinta Basin. Our undisturbed soil flux measurements were not adequate to quantify rates of natural hydrocarbon seepage in the Uinta Basin.