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Littered cigarette butts as a source of nicotine in urban waters
Amy L. Roder Green
a
, Anke Putschew
b
, Thomas Nehls
a,
⇑
a
Technische Universitaet Berlin, Chair of Soil Conservation, Ernst-Reuter-Platz 1, 10587 Berlin, Germany
b
Technische Universitaet Berlin, Chair of Water Quality Control, Strasse des 17. Juni 135, 10623 Berlin, Germany
article info
Article history:
Available online xxxx
Keywords:
Nicotine
Cigarette butts
Surface run-off
Urban waters
Drinking water contaminant
Urban litter
summary
The effect of nicotine from littered cigarette butts on the quality of urban water resources has yet to be
investigated. This two-part study addresses the spatial variation, seasonal dynamics and average resi-
dence time of littered cigarette butts in public space, as well as the release of nicotine from cigarette butts
to run-off in urban areas during its residence time. Thereby, we tested two typical situations: release to
standing water in a puddle and release during alternating rainfall and drying. The study took place in
Berlin, Germany, a city which completely relies on its own water resources to meet its drinking water
demand. Nine typical sites located in a central district, each divided into 20 plots were studied during five
sampling periods between May 2012 and February 2013. The nicotine release from standardized ciga-
rette butts prepared with a smoking machine was examined in batch and rainfall experiments.
Littered cigarette butts are unevenly distributed among both sites and plots. The average butt concen-
tration was 2.7 m
2
(SD = 0.6 m
2
,N= 862); the maximum plot concentration was 48.8 butts m
2
. This
heterogeneity is caused by preferential littering (gastronomy, entrances, bus stops), redistribution
processes such as litter removal (gastronomy, shop owners), and the increased accumulation in plots
protected from mechanized street sweeping (tree pits, bicycle stands). No significant seasonal variation
of cigarette butt accumulation was observed. On average, cigarette butt accumulation is characterized by
a 6 days cadence due to the rhythm and effectiveness of street sweeping (mean weekly butt accumula-
tion rate = 0.18 m
2
d
1
; SD = 0.15 m
1
). Once the butt is exposed to standing water, elution of nicotine
occurs rapidly. Standardized butts released 7.3 mg g
1
nicotine in a batch experiment (equivalent to
2.5 mg L
1
), 50% of which occurred within the first 27 min. In the rainfall experiment, the cumulative nic-
otine release from fifteen consecutive precipitation events (each 1.4 mm) was 3.8 mg g
1
, with 47% dur-
ing the first event. According to these results, one cigarette butt may contaminate an amount of 1000 L
water to concentrations above the predicted no effect concentration (PNEC) of only 2.4 10
3
mg L
1
(Valcárcel et al., 2011). Given the continuous littering of cigarette butts, and the rapid release of nicotine,
cigarette butts are assessed to be a relevant threat to the quality of urban waters and consequently to
drinking water.
Ó2014 Elsevier B.V. All rights reserved.
1. Introduction
One of the most common elements of urban litter, a cigarette
butt, contains a complex mixture of toxins, including the highly
water-soluble nicotine. Extremely addictive, nicotine is consumed
in massive amounts around the world: 20% of the population over
15 years of age smoke on average 16 cigarettes per day (Giovino
et al., 2012). With 73% of the world’s population over the age of
14 years (United Nations, online), worldwide an estimated 16 bil-
lion cigarettes are consumed daily. With an estimated urbanization
of 60% in 2030 (United Nations, online) about 10 billion cigarettes
will then be smoked in urban areas every day.
Cigarette butts are the most commonly littered item in urban
areas (Bator et al., 2011; Schultz et al., online), making up
22–46% of visible litter, as reported in numerous litter audits
worldwide (Schneider et al., 2011; Seco Pon et al., 2012;
Moriwaki et al., 2009; Schultz et al., online). Patel et al. (2013)
observed that in cities, 76% of cigarettes smoked in public were lit-
tered, rather than disposed in appropriate receptacles. The butts
are then transported by urban waters to other ecosystems such
as coastal areas, where they are consistently the most numerous
element of litter collected (International Costal Clean-up, 2013;
Ariza et al., 2008). The persistence of cigarette butt filters, made
of non-biodegradable cellulose acetate is a concern for wildlife
http://dx.doi.org/10.1016/j.jhydrol.2014.05.046
0022-1694/Ó2014 Elsevier B.V. All rights reserved.
⇑
Corresponding author. Tel.: +49 (0)30 314 73539; fax: +49 (0)30 314 23309.
E-mail address: thomas.nehls@tu-berlin.de (T. Nehls).
Journal of Hydrology xxx (2014) xxx–xxx
Contents lists available at ScienceDirect
Journal of Hydrology
journal homepage: www.elsevier.com/locate/jhydrol
Please cite this article in press as: Roder Green, A.L., et al. Littered cigarette butts as a source of nicotine in urban waters. J. Hydrol. (2014), http://dx.doi.org/
10.1016/j.jhydrol.2014.05.046
(Stanley et al., 1988). Cigarette butts are thus a concern in terms of
its environmental, public health, social, and economic conse-
quences (Marais and Armitage, 2004b; Pon et al., 2012; Schultz
et al., 2013; Schneider et al., 2011).
Cigarette butts are not evenly distributed in the urban environ-
ment. Distribution of butts is linked to the location of sales and
consumption. The highest concentrations in the US are associated
with bars, convenience stores, liquor stores, cafés, gas stations, gro-
cery stores, restaurants, and traffic signals (Marah and Novotny,
2011). A preference of cigarette smoking has been observed in con-
junction with alcohol, coffee, meals, and during breaks, (Van Gucht
et al., 2010). Cigarette butts are discarded at places of transition
from an outdoor to an indoor environment where smoking is not
tolerated, such as entrances to buildings, vehicles or public trans-
portation stations, where the authors found a cigarette butt con-
centration of 102 m
2
in one puddle (see Fig. 1). Non-smoking
legislation, in effect in Berlin since 2008, prohibits smoking in
the indoor workplace, inside public transit stations and platforms,
restaurants, and bars. Since then, it is more common to see an
accumulation of smokers outside of restaurant entrances and offi-
ces. This phenomenon may well have caused an increase of littered
cigarette butts to the urban environment.
The quality of urban run-off is linked to urban litter (Marais
et al., 2004a), which in turn is recognized as a major threat to
urban water quality (Heinzmann, 1998).
1.1. Nicotine toxicity
Cigarette butts contain a mixture of substances with toxic
effects to organisms, most notably heavy metals, polycyclic aro-
matic compounds, ethyl phenol, and nicotine (Micevska et al.,
2006; Moerman and Potts, 2011; Moriwaki et al., 2009). The
human toxicological and health effects of nicotine have been
extensively studied (Brc
ˇic
´Karac
ˇonji, 2005). Nicotine is easily
absorbed through the skin, lung alveoli, small intestine, and
urinary bladder. It passes easily through the placenta to the fetus.
Strong teratogenic and genotoxic effects have been observed. Nic-
otine is associated with cardiovascular disease and acts on the cen-
tral nervous system. Acute toxicity causes death due to paralysis of
respiratory muscles or respiratory failure. Nicotine is known to
cause liver damage in fish (Konar, 1970), and effects planarians
in a similar way as in mammals (Rawls et al., 2011). The effects
of chronic sub-lethal concentrations of nicotine and its metabolites
in the aquatic environment are not well understood. Based on the
EC50 for Daphnia of 0.2 mg L
1
(Savino and Tanabe, 1989), the cal-
culated value of the predicted no effect concentration (PNEC) for
nicotine is 2.4 10
3
mg L
1
(Valcárcel et al., 2011).
1.2. Nicotine in water resources
Nicotine, and its most important metabolite, cotinine, are
important emerging pollutants, widely detected in water resources
worldwide in studies of pharmaceutically active compounds
(Stuart et al., 2012; Benotti and Brownawell, 2007; Focazio et al.,
2008; Valcárcel et al., 2011). Littered cigarette butts have not been
examined to date as a source of nicotine in urban waters.
Nicotine has been in use as an insecticide since the 15th cen-
tury. Because of its toxicity to aquatic organisms, its application
has been severely limited in the US, Canada and Europe. Today, nic-
otine is on the toxic release inventory (TRI) in United States, thus
its release into the environment must be reported to state author-
ities (Environmental Protection Agency, 1996). The European
Union classifies tobacco waste as toxic and hazardous when the
nicotine content exceeds 0.5 mg g
1
dry weight (Civilini et al.,
1997). The nicotine content of cigarettes varies according to brand
and country of consumption. Between 1998 and 2005, the mean
concentration of nicotine in the tobacco rods sold by major manu-
facturers increased by 9% from 17.1 mg g
1
to 18.7 mg g
1
in the
USA (Connolly et al., 2007).
Nicotine has been identified as one of the three most significant
pharmaceuticals with regard to the potential eco-toxicological and
toxicological impacts of waste-water treatment plant (WWTP)
effluent (Muñoz et al., 2008). In an extensive study of emerging
pollutants in Madrid, Spain, nicotine was detected in all river
samples downstream from WWTP, with concentrations of up to
1.9 10
3
mg L
1
(Valcárcel et al., 2011). Leaking septic tanks have
been linked to nicotine concentrations of up to 8.1 10
3
mg L
1
in
UK groundwater (Stuart et al., 2012). Nicotine concentrations rang-
ing from 2.5 to 6 10
4
mg L
1
were observed in estuary water in
the US in the proximity of a WWTP (Benotti and Brownawell, 2007).
Nicotine is also found in drinking waters worldwide. An
international study in 30 cities reported an average nicotine
concentration of 1.9 10
5
mg L
1
(Boleda et al., 2011). In Madrid,
Spain, nicotine was detected in 3 of 5 of tap water samples at levels
higher than 4 10
6
mg L
1
reaching up to 1 10
4
mg L
1
(Valcárcel et al., 2011). In Miami, USA, concentrations of nicotine
of 3 10
3
mg L
1
have been observed, thus clearly above the
PNEC (National Research Council, 1977).
Even in bottled mineral water taken from pristine aquifers, far
from anthropogenic sources or sites of tobacco cultivation or
production, nicotine was detected in concentrations of up to
1.5 10
5
mg L
1
(Alonso et al., 2012).
It is important to understand sources, pathways and transfor-
mations of nicotine at the numerous natural and technical urban
water interfaces (Gessner et al., 2014) and its relevance as an urban
water contaminant. As littered cigarette butts may be one of these
sources, the aims of the study are:
(i) To analyze the spatial and temporal variation of littered
cigarette butt accumulation in Berlin, Germany, and to
determine average butt weights and residence times, as
well as.
Fig. 1. Typical situation at the entrance of an underground station in detail.
Cigarette butt count in the 1.44 m
2
area in the puddle tallied 151. (Photo: T. Nehls,
taken on 27.11.2012 in Berlin, Germany).
2A.L. Roder Green et al. / Journal of Hydrology xxx (2014) xxx–xxx
Please cite this article in press as: Roder Green, A.L., et al. Littered cigarette butts as a source of nicotine in urban waters. J. Hydrol. (2014), http://dx.doi.org/
10.1016/j.jhydrol.2014.05.046
(ii) To investigate the elution of nicotine from average cigarette
butts in average residence times in a batch and a simulated
rainfall experiment, simulating elution in standing water
and during rainfall and drying cycles.
By combining results from the two studies (iii) we assess if cig-
arette butts are a significant source of nicotine in surface run-off
and surface waters in the urban context. Recommendations for city
planners are then discussed.
2. Materials and methods
2.1. Sites and cigarette butt sampling
The study was conducted in Berlin, Germany, with a resident
population of 3.5 million, and 9.7 million visits from tourists in
2011. It is estimated that 31% of the Berlin residents are cigarette
smokers (Amt für Statistik Berlin-Brandenburg, online), which is
higher than the worldwide average. The average population den-
sity in the inner-city study area is 11,150 person km
2
, the highest
among German inner-city areas (Umweltatlas Berlin, online).
Preliminary samplings were conducted in various areas of the
city which in part confirmed spatial patterns of littered cigarettes
as reported by Marah and Novotny (2011), and from which we
derived criteria for site selection. As representativeness is difficult
to achieve in urban areas, and because of limited resources, we
chose the study area which represented the widest range of
land-use types, human impact intensities, and cigarette littering
frequencies expected within an inner-city district. Furthermore,
the area included combined and separate sewage systems, and
open soil, as these features indicate differing nicotine pathways
to surface water bodies and groundwater. The city of Berlin relies
on water resources from within the city limits for 100% of its drink-
ing water supply.
The inner-city area Treptow–Kreuzberg was identified to be an
appropriate fit for the above mentioned criteria. The area is
average in relation to socio-economic indicators such as property
values, and unemployment rate (fis Berlin, online). The 1.8 km
2
study area includes typical urban land use types such as mixed res-
idential (apartments, town houses), commercial (office space,
small businesses like tobacco shops, barber shops), public trans-
port (metro station, train station and bus stops), and a variety of
gastronomy types (bistro, restaurant and fast food). The quarter
is in close proximity to the receiving urban water bodies, the river
Spree and the canal Landwehrkanal. Nine sites with a total sam-
pling area of 1955 m
2
were selected within the study area and
were sub-divided into plots (see below). The individual sites were
not chosen based on the proportional representativeness of a larger
city area. Rather, sites were chosen to represent a wide range of
expected littering, from hotspots to sites with very small littering
frequency (based on preliminary samplings and observations).
The expected high concentration areas included public transit
hubs, intensive night-life locations, and office space, while low
concentration sites included quiet residential areas with no com-
mercial use, and with low pedestrian frequency. A summary of site
information is provided in Table 1.
2.1.1. Plot design
At each site, twenty plots (one site had 21 plots) of variable size
>3 m
2
(average 10.8 m
2
,N= 181, SE = 0.4 m
2
) were demarcated on
the sidewalk. The intention of the plot design was to investigate
the spatial distribution of cigarette butts according to the features:
tree pits (sites 1, 2, 3, 4, 5), bus stops and their waiting areas (sites
1, 7, 8, 9), bike stands, entrances to buildings, shops, or properties
(all sites), and gastronomy including restaurants, fast-food stands,
convenience stores and bars (sites 1, 5, 6, 8). All features were stud-
ied across varying intensities of human impact, and thus cigarette
littering. Based on observations, the plots were also demarcated to
include site-specific local pockets of high cigarette accumulation in
order to assess worst case situations. The variance in the plot sizes
is due to the heterogeneity of the studied sites and features. Plots
with the feature tree pit contained, in addition to the unpaved area
itself, the row of pavement stones bordering the tree pit. All plots
adjacent to the street included a 0.1 m strip of the adjoining gutter.
The goal of investigating a widest possible range of cigarette
butt concentrations, including worst case scenarios, implies a cer-
tain sampling bias. However, due to the large number of plots
(N= 181), this sampling design is well-suited for an analysis of
the spatial patterns and accumulation trends, rather than a repre-
sentative magnitude for central Berlin.
2.1.2. Sampling scheme
A total of five collections were conducted between May 2012
and February 2013. All sites were investigated for variations in
short term (1–3 weeks) and long term (13–17 weeks) accumula-
tion periods, as well as seasonal variation. The accumulation period
is defined as the number of days between sampling events in
which new cigarette butts are accumulated in the plots. At collec-
tions, all identifiable cigarette butts, including damaged or extre-
mely weathered pieces found within plots were removed from
the site (sometimes getting pitying looks and fresh cigarettes been
offered) and brought to the laboratory. They were then counted,
some were dried (50 °C), and weighed (average butt weight of
0.2 g, N= 4,787). Differences in accumulation periods lengths were
due to extreme weather situations such as heavy rain, snowstorms,
or long periods of remaining ice and snow in which it was impos-
sible to find and collect all cigarette butts from all plots of the sites.
2.1.3. Data analysis – butt collection
Statistical analysis of the data was performed using R software
(Version 2.15.2, R Development Core Team). Means of cigarette
butt concentrations for the plots were not normally distributed
when tested on each sampling (Shapiro–Wilk test p< 0.05). As nor-
mal distribution was not achieved through data transformation,
statistical analysis of the significant difference of the means
according to the features described above, was performed using
the non-parametric Kruskal Wallis test. Requirements of homoge-
neity of variances were tested with the Fligner Kileen test. For the
features bus stop, entrance, bicycle stand, and gastronomy, only
plots containing the feature were counted as such. Features with
significant differences in means were compared against one
another via plot means, normed over site and sampling. These
means, with normal distributions and homogeneous variances,
were then tested with ANOVA, and Tukey post hoc tests.
For the analysis of temporal distribution, it was necessary to
compare butt accumulation across all sites with differing concen-
tration ranges. Therefore, the site means were normed by the high-
est plot concentration across all collection periods. The site means
were then grouped according to accumulation period and plotted.
To analyze the accumulation dynamic of cigarette butts in plots
with special features, all plots were grouped by feature, and then
the concentrations were normed by the highest plot concentra-
tions over all collection periods in the groups.
2.2. Nicotine elution from cigarette butts
The collections in the city described above were designed to
determine the variability and average concentrations, butt weights
and residence times, while in the laboratory experiments,
described in the following, the nicotine release from average ciga-
rette butts during the resulting residence times was determined.
A.L. Roder Green et al. / Journal of Hydrology xxx (2014) xxx–xxx 3
Please cite this article in press as: Roder Green, A.L., et al. Littered cigarette butts as a source of nicotine in urban waters. J. Hydrol. (2014), http://dx.doi.org/
10.1016/j.jhydrol.2014.05.046
2.2.1. Preparation of standardized cigarette butts (SCBs)
‘Standardized cigarette butts’ (SCBs) used in the study were
produced in the laboratory from the cigarette brand with the
highest worldwide market share (Mackay and Ericksen, 2002)
purchased in Berlin, Germany. The nicotine content of this product
was close to the mean of all products with over 3% market share in
the US (Kozlowski et al., 1998).
The average cigarette butt length of 3.7 10
2
m(N= 124) was
ascertained from freshly discarded cigarettes from an extra
sampling campaign which corresponded to a SCB’s dry weight of
0.3 g (N= 8). All SCBs were smoked to this length with a smoking
machine (RM 20/CS; Heinrich Borgwaldt GmbH, Hamburg,
Germany) according to ISO 3308:2012 (puff volume: 35 ± 0.3 mL,
puff duration: 2 ± 0.05 s, puff frequency: 60 ± 0.5 min
1
). Addition-
ally, SCBs with 3, 6, and 7 10
2
m length were produced. The
SCBs were dried at 50 °C prior to use in the following laboratory
experiments.
2.2.2. Batch experiment puddle
In order to study the release of nicotine from cigarette butts,
one SCB was added to 1 L of purified water in an amber glass bottle
(three replicates). Aliquots of 0.01 L were taken after 0.5, 10, 30, 60,
90, 120, 240, 1440 min, filtered with a 0.45
l
m glass fiber mem-
brane (GFM Whatman) and stored at 4 °C before analysis. Prior
to sampling, the bottle was inverted two times. This minimal
amount of mixing was employed to avoid a physical disintegration
of the cigarette butt, and to make the release comparable to the
situation in a puddle, thus resulting in a conservative estimation
of release. The volume decrease due to sampling was considered
in the calculation of concentrations.
In order to investigate the relationship between butt length
and the nicotine release, the batch experiment was repeated
(t= 240 min, see below) with SCB of 3, 6, and 7 10
2
m and 0.2,
0.5, 0.6 g respectively. Then the released nicotine was related to
the SCB weights and to the tobacco weight in the SCB (cigarette
filters alone were 2.1 10
2
m and weighed 0.17 g).
2.2.3. Simulated rainfall experiment
Five SCBs were weighed and distributed on a stainless steel tray
(0.16 m
2
) with a 2% slope (usual sidewalk slope). The tray was
mounted on top of a continually logged scale (Fig. 2). The SCBs
were exposed to 15 consecutive simulated daily rainfall events
with an average flow rate of 0.18 mm min
1
, and an average sum
of 1.44 mm d
1
. This event sum is less than 5% of the precipitation
event distribution in Berlin (Nehls et al., 2011), and thus an esti-
mate of the minimum amount of water which comes into contact
with littered cigarette butts.
Daily run-off from the tray was collected, and stored in amber
glass bottles at 4 °C. After the 15 rainfall events, the SCBs were
removed, dried at 50 °C, and weighed. Remaining nicotine was
eluted from each SCB in 0.25 L of de-ionized water for 1440 min
(sampling described above).
2.2.4. Analysis of nicotine in water
Nicotine was quantified using LC positive-ESI–MS/MS (HP 1100,
Agilent, Waldbronn, Germany; Quattro Micro, Waters). Nicotine
was detected in the selected reaction monitoring (SRM) mode. The
product ions for the SRM experiments were determined by infusion
of nicotine (product ions m/z117 and 130), and continine-d
3
(prod-
uct ions m/z101 and 80) which was used as an internal standard. For
both compounds the cone voltage was set to 30 V and the collision
energy to 23 V. The pressure in the collision cell was 1.95 10
6
bar. Ultrapure water and methanol, both with 1 10
3
M ammo-
nium acetate, were used as an eluent for the LC separation The
following elution was employed: initial 90% water isocratic for
0.5 min, a linear gradient to 100% methanol within 2.5 min, and then
within 0.5 min to 90% water which was isocratic for 16.5 min. The
flow was 2.5 10
3
L min
1
and the column was set to 30 °C.
The compounds were analyzed with 5 10
5
L of the internal
standard added to 1 10
3
L of each sample. The concentration
was determined from the peak area ratio of m/z117 (nicotine) to
m/z80 (continine-d
3
). The mass spectrometer was calibrated from
50 to 800 10
6
gL
1
nicotine with correlation coefficients
greater than 0.998. The limit of quantification, determined by
preliminary analysis, is 4 10
5
gL
1
nicotine. All samples were
analyzed twice.
Table 1
Description of the sites for littered cigarette butts collection in Berlin, Germany.
Site no. Address Type of use Latitude Longitude Functional features
1 Lohmühlenplatz Residential 52°29
0
21.64
00
N13°26
0
26.27
00
E bu, en, ga, tp
2 Lexisstrasse Residential 52°29
0
25.48
00
N13°26
0
30.68
00
E en, tp
3 Martin-Hoffmann Strasse Residential 52°29
0
42.94
00
N13°27
0
26.12
00
E en, tp
4 Martin Hoffmann Strasse Office 52°29
0
40.57
00
N13°27
0
33.21
00
E bst, en, tp
5 Schlesische Strasse Residential/nightlife 52°29
0
59.04
00
N13°26
0
39.20
00
E bst, en, ga, tp
6 Treptower Park S-Bahn Station Public transport 52°29
0
35.69
00
N13°27
0
38.52
00
E bst, en, ga
7 Elsenstrasse Public transport 52°29
0
32.46
00
N13°27
0
29.37
00
E bst, bu, en, tp
8 Schlesische Strasse Public transport 52°29
0
51.48
00
N13°26
0
52.80
00
E bu, en, ga
9 Reichenberger Strasse Public transport 52°29
0
37.23
00
N13°26
0
13.50
00
E bu, en, tp
tp – tree pit, unpaved sidewalk vegetation, bu – bus-stop, en – entrance including commercial, residential, office, or fenced yard, ga – gastronomy, bs – bicycle stand.
a
b
d
e
c
f
h
g
Fig. 2. Experimental setup for the rainfall simulation (a) Mariott’s bottle, (b) needle
irrigator, (c) hermetically sealed plexiglas box, (d) data logger, (e) stainless steel
tray with standardized cigarette butts, (f) digital scale, (g) run-off collection, and (h)
pressure difference, adjusted to the targeted rainfall rate.
4A.L. Roder Green et al. / Journal of Hydrology xxx (2014) xxx–xxx
Please cite this article in press as: Roder Green, A.L., et al. Littered cigarette butts as a source of nicotine in urban waters. J. Hydrol. (2014), http://dx.doi.org/
10.1016/j.jhydrol.2014.05.046
Nicotine and continine-d
3
were purchased from Sigma Aldrich.
7.92 10
5
L nicotine (density 1.010 g cm
3
) was dissolved in
0.1 L ultra pure water, and than diluted to final concentrations of
80, 50, 40, 20, 10 and 5 10
2
mg L
1
. Continine-d
3
(1 g L
1
in
methanol) was diluted to the final concentration of 1 10
3
gL
1
with ultrapure water. The ultrapure water was produced from
de-ionized water with a water purification system (maxima ultra-
pure water; Elga, Upstadt-Weiher, Germany). All other chemicals
used (methanol, ammonium acetate) were LC–MS quality.
3. Results and discussion
3.1. Spatial variation of littered cigarette butts in Berlin
The mean butt concentration over all collections and sites is
2.7 m
2
(SD = 0.64 m
1
,N= 862 sampled plots). The lowest site
mean, 0.29 m
2
(SD = 0.15 m
2
), was observed at site No. 2, a quiet
residential side street, with a low pedestrian frequency, as well as
an absence of any businesses or public transit stops. The highest
mean, 5.2 m
2
(SD = 2.2 m
2
), was observed at site No. 6, at the
main entrance to a well-frequented city train station, including
convenience stores, fast food, and bicycle stands.
The spatial distribution of cigarette butts is characterized by
pockets of high concentration, on all scales (within the study area,
within sites and within plots). Thus, all sites are characterized by a
similar right skewed frequency distribution of plot concentrations
(Fig. 3). The highest concentration of littered cigarette butts in a
single plot was found in site No. 6 near a train station entrance
with 48 m
2
. That corresponds to a number of 581 butts, almost
all of which were concentrated in a large pile of snow. This is an
exceptionally high number, most probably containing butts, which
were transferred from other plots, or from areas outside the study
site. This data has been included in the analysis as it depicts an
observed concentration in one plot. This number is relevant for
the ecological effects of cigarette butts, regardless of whether the
cigarette butts were originally discarded there, or transported
through snow removal and sweeping at a later point. Accordingly,
individual plot concentrations are up to 500 times higher than the
respective mean (Fig. 3). Effects such as wind, water, pedestrians,
street sweeping, or snow removal, as well as preferential littering,
lead to very heterogeneous distributions of butts in certain plots.
There will always be limited certainty as a dynamic system like
the city may change while being sampled.
The means of plot concentrations grouped by features are sig-
nificantly different for all samplings (Kruskal Wallis of normed plot
concentrations, p< 0.05). The Tukey post hoc test showed that only
tree pits contain significantly more (2.9 times more) littered ciga-
rette butts than the control plots with none of the special features
(Fig. 4). Tree pits are not cleaned regularly by mechanized street
sweeping. Whether butts are preferentially littered to tree pits or
the concentration is enriched relative to the surrounding area is
not clear. That cigarette butts are removed from other plots and
put into tree pits by the sweeping cannot be excluded.
The cigarette butt concentration in bus stops is not significantly
lower than in tree pits. Although it is 1.9 times higher than in con-
trol plots, that difference is not significant. In winter, when people
use public transit more frequently, we observed a trend of higher
concentrations. The feature bus stop was not mentioned as a
cigarette butt accumulation hotspot in a US American study
(Marah and Novotny, 2011). Public transport is more important
in Germany, and thus it explains spatial distribution of urban litter
to a higher extent than in the USA.
Bicycle stands seem to be protected from sweeping in the same
way as tree pits. Means of normed butt concentrations are 1.5
times higher than that of the control plots. The predominant group
of bicycle stands was located in site No. 6 near the entrance to a
city train station. This uncovered bicycle parking area was not well
maintained, and contained a large amount of garbage, fallen leaves,
and abandoned bicycles. Littering rates are known to be higher in
areas where litter is already present (Schultz et al., 2013). The plot
concentrations of the bicycle stands in site No. 6 were especially
high for the last winter collection, in which snow had been pushed
into large piles.
The feature gastronomy includes restaurants, a fast-food stand,
a convenience store, and bars. Therefore it includes many of the
types of land use associated with increased butt concentrations
in the study from Marah and Novotny (2011). Our results do not
show this feature to be the most important indicator of butt con-
centrations. We observed that not all of the business owners sweep
the area in front of their business on a daily basis. Some proprietors
dispose the butts properly, while others sweep the butts into the
gutters or tree pits. Thus, heterogeneous sweeping activities
change the spatial patterns of littered cigarettes leading to both
higher accumulation in specific areas, as well as a lower accumula-
tion due to the removal of cigarette butts from the street into prop-
erly treated waste streams.
Most probably for the same reasons, plots with the feature
‘entrance’ did not differ at all from the control plots when analyzed
Sites
Littered cigarette butts [m-2]
12 34 56 78 9
0
10
20
30
40
50
Fig. 3. Concentration of littered cigarette butts for all samplings in all plots of sites
1–9, Berlin, Germany.
Fig. 4. Concentrations of littered cigarette butts normed by the highest concentra-
tion per site, and grouped by functional features. Columns depict arithmetic means,
error bars depict the standard error. Bars labeled by the same letter are not
significantly different (p< 0.05, N= 181 plots).
A.L. Roder Green et al. / Journal of Hydrology xxx (2014) xxx–xxx 5
Please cite this article in press as: Roder Green, A.L., et al. Littered cigarette butts as a source of nicotine in urban waters. J. Hydrol. (2014), http://dx.doi.org/
10.1016/j.jhydrol.2014.05.046
across all samplings and sites. The feature entrances, like the fea-
ture gastronomy, are composed of a non-homogenous group of
plots next to a doorway, gated yard, or an entrance to a train sta-
tion. Some plots were located at entrances to small businesses such
as a hairdresser, or a driving school. The workers in these busi-
nesses were observed to smoke outside their workplaces during
breaks. The high numbers of cigarette butts collected in site No.
4, are due to the entrance to an office space, where many employ-
ees take their breaks outside with a cigarette. Although people toss
cigarettes before going back to work, they do not necessarily drop
the cigarette butt directly at the entrance. Butts can be flicked wide
distances away from entrances, or dropped some meters in front of
the entrance.
Furthermore, we observed that cigarette butts tend to accumu-
late in large or uneven pavement joints, such as in cobblestone
pavements. In smooth pavement with narrow joints, fewer ciga-
rette butts accumulate.
3.2. Temporal variation of littered cigarette butts in Berlin
Cigarette butts are continually littered into the urban environ-
ment. A seasonal variation was not significantly indicated from
our samplings. This finding corresponds with other studies on
urban litter (Seco Pon et al., 2012). There was also no difference
in cigarette butt concentrations between short and long term accu-
mulation periods, exemplified by the oscillating pattern of the
temporal variation in Fig. 5a. Despite the great variability between
the plots, the average residence time over all sites is six days, as
derived by analyzing the phases in which the number of butts
increased (5, 4, 6, 6, 9 days). This corresponds to the sweeping
frequency by municipal agencies which – depending on the site
– varies from a weekly to a daily rhythm (such as at the train sta-
tion, Berliner Stadtreinigung GmbH, personal information and own
observation). Some business owners, as discussed above, also
sweep on a daily basis, thus we conclude a minimum accumulation
period or residence time of littered cigarette butts of one day. On
average, littered cigarette butt accumulation is characterized by a
six days cadence with an average butt accumulation rate of
0.18 m
2
d
1
; SD = 0.15 m
1
d
1
.
For the feature tree pit (Fig. 5b), there is a trend of higher accu-
mulation with larger sampling intervals. The accumulation periods
are longer than for all plots. Thorough cleaning by manual munici-
pal sweeping occurs a few times per year, resulting in the removal
of almost all butts in tree pits and bike stands (Berliner Stadtreini-
gung GmbH, personal information).
Furthermore cigarette butts are littered continuously, but they
are not littered consistently. Some areas will experience littering
during working hours, as in areas outside of offices, schools, or
small businesses, while other areas will see more littering on
weekends and at night.
We conclude that the distribution of butts is characterized by
site specific short term patterns of increase and decrease due to
littering, weathering, erosion, removal and re-distribution with a
minimum residence time of one day. The dynamic of nicotine
release from a littered cigarette butt is discussed in the following
section.
3.3. Nicotine release from standard cigarette butts
The batch experiment is a realistic description of the elution
dynamic when cigarette butts come into contact with standing
water, including permanent bodies of water such as a lake or a
river, but also puddles in street or sidewalk depressions caused
by precipitation. In the batch experiment, 7.1 mg g
1
(SD = 0.07
mg g
1
) nicotine was released from the SCB after 1440 min, 50%
of the total amount after 27.2 min and 90% already after 651 min
(Fig. 6a). The released concentration after 1440 min is therefore
considered to be the total releasable nicotine from SCBs for the
rainfall experiment. Nicotine is released quickly to the water
phase, according to a first order reaction model C
L
= 0.98 ln
(t) + 0.65 (R
2
= 0.94) with C
L
the soluble nicotine concentration
(mg g
1
) and tthe reaction time (min).
Surprisingly, the nicotine release (mg g
1
) from cigarette butts
increases according to butt weight M
SCB
(C
L
=19 M
SCB
+ 0.5;
R
2
= 0.92). This is due to the fact, that the nicotine release from
the butt is determined by the remaining tobacco (constant at
16.2 mg g
1
tobacco; SD = 1.6 mg g
1
,N= 12) instead of the filter
(0.22 mg g
1
filter).
The water-extractable amount of nicotine from a SCB is 14
times higher than the threshold established by the European Union
for hazardous tobacco waste (0.5 mg g
1
)(Civilini et al., 1997).
From such puddles, nicotine may enter the groundwater, from
which drinking water is extracted in Berlin. The filtration capacity
of paved soils is decreased depending on the pavement and
sub-soil permeability function, as well as the susceptibility to pref-
erential flow, (Nehls et al., 2008). Nicotinophilic micro-organisms
Fig. 5. (a) Concentrations of littered cigarette butts normed by the highest value for the site in all samplings in relation to the sampling intervals for all plots (N= 862 plots)
and (b) plots with tree pits. Squares and diamonds depict arithmetic means, error bars depict standard errors (N= 102 plots).
6A.L. Roder Green et al. / Journal of Hydrology xxx (2014) xxx–xxx
Please cite this article in press as: Roder Green, A.L., et al. Littered cigarette butts as a source of nicotine in urban waters. J. Hydrol. (2014), http://dx.doi.org/
10.1016/j.jhydrol.2014.05.046
capable of nicotine degradation in water (Civilini et al., 1997) and
soils (Ma et al., 2012) have been identified. The existence and activ-
ity of such micro-organisms in the particular environment of pave-
ment joint soils (Nehls et al., 2006) have not yet been investigated.
Standing water is common in historic quarters of cities, but not
the rule. Therefore, we also tested the elution of nicotine from
butts exposed to rainfall without puddle formation.
In the simulated rainfall experiment, the cumulative total nico-
tine elution from SCBs was 3.8 mg g
1
from a total precipitation of
21.6 mm in fifteen events (Fig. 6b). Half of the nicotine was eluted
after 1.6 mm or 1.1 events. Again, a first order reaction model pro-
vides a good description of the elution dynamic: C
L
= 0.79
Ln(P) + 1.62 (R
2
= 0.90), with Pthe sum of rainfall [mm]. Based on
the results of the batch experiment, we recovered a sum of 55% of
the total water-extractable nicotine in the SCB’s. The remaining
amount of nicotine in the SCBs after the 15 rainfall events was
0.16 mg g
1
(SD = 0.02 mg g
1
;N= 5). It can be concluded, that
even cigarettes, which were exposed to several precipitation events
(in our case seven events) must be classified as hazardous waste.
The measured nicotine concentrations in the run-off water
reached up to 5.3 mg L
1
g
1
SBC. Applied to the mean butt concen-
tration of the study area, nicotine concentrations in the run-off are
estimated to reach 0.62 mg L
1
(1.44 mm rain event, run-off
coefficient = 1). Local concentrations can be as high as 11.4 mg L
1
calculated using the highest observed plot concentration. Both con-
centrations are far above the PNEC, (2.4 10
3
mg L
1
)(Valcárcel
et al., 2011), as well as the EC50 for Daphnia (0.2 mg L
1
)(Savino
and Tanabe, 1989). As cigarette butts are continuously and copi-
ously littered in the urban environment, and given the rapid elution,
every precipitation event will release relevant amounts of nicotine
into the urban environment. The high local concentrations in hot
spots can lead to nicotine flushes, a concern for aquatic ecosystems.
Obviously, nicotine concentrations in surface run-off may be
extreme for small rain events. Surface run-off draining to separate
sewer systems leads directly into surface water bodies without
treatment. Effluent from WWTP and leaking septic systems are
assumed to be the main source of nicotine contamination in surface
and ground water. As nicotine elimination in WWTP has been
observed at rates of 75–99% efficiency (Huerta-Fontela et al.,
2008), the contribution of nicotine from paved urban areas should
be considered as a source of nicotine in surface waters.
While the reported data and calculations are based on experi-
mental study of one common cigarette brand, real-world cigarette
litter consists of a mixture of brands and products with varying
nicotine content. As more nicotine is contained in the tobacco than
in the filter of cigarette butts, the released nicotine depends on the
behavior of smokers with regard to littered butt length (weight,
filter to tobacco ratio). Likewise, littering habits depend on cultural
and socio-economic factors beyond the scope of this study. Conse-
quently nicotine elution will vary due to the local preferences of
smokers, as well as the behavior (littering and sweeping) of resi-
dents and municipalities. Herein lays the key to cope with the
problem!
4. Conclusions and implications for city planning
This study demonstrates that (i) cigarette butts accumulate in
high numbers in urban areas and (ii) the nicotine which is released
from such litter poses a significant threat to urban water resources.
Cigarette butts are continuously littered into the urban environ-
ment, and accumulate in areas where they are not regularly
removed by private or municipal actors (e.g. tree pits). First flush
events with high nicotine concentrations are likely to take place
after longer accumulation periods with dry weather. Each littered
cigarette butt can potentially release nicotine in concentrations
higher than the threshold value of hazardous and toxic waste
defined by the European Union. Having its nicotine fully released
to standing water, only one cigarette butt can contaminate an
amount of 1000 L water to concentrations above the predicted no
effect concentration (PNEC) of only 2.4 10
3
mg L
1
(Valcárcel
et al., 2011).
Thus, municipalities have a legal obligation to make sure that
this tobacco waste is disposed in an appropriate way. One
approach, suggested by Novotny et al. (2009), is to hold cigarette
companies legally responsible. Regardless of legal or financial
responsibility, management of cigarette butt littering in cities must
be implemented.
Although a more effective and frequent street sweeping would
help to reduce the released amount of nicotine, our study shows
that the present system is already effective where it reaches the lit-
ter. It is questionable, if higher frequencies of mechanized street
sweeping would change the situation in the high accumulation
pockets significantly.
Increasing the number of public ashtrays in areas with high cig-
arette butt concentrations, such as near well-frequented areas, and
bus stops, could reduce cigarette butt littering. Although public
ashtrays are already installed on top of the numerous public trash
receptacles in the city of Berlin, cigarette butts are littered in large
0
2
4
6
8
0 360 720 1080 1440
time [min]
released nicotine [mg g-1butt]
nicotine in water [mg L-1 g-1butt]
0
1
2
3
4
01020
cumulative sum of rainfall events [mm]
released nicotine [mg g-1 butt]
1
2
3
4
5
6
7
8
nicotine [mg L-1g-1 butt]
cumulative released
nicotine in water
first order reaction model
nicotine
first order reaction model
ab
Fig. 6. (a) Dynamic of nicotine release from standardized cigarette butts to water in batch experiments and (b) dynamic of nicotine release from standard cigarette butts to
water in a series of simulated rainfall events in the laboratory (right). Circles and diamonds depict arithmetic means, error bars depict standard errors (N= 3).
A.L. Roder Green et al. / Journal of Hydrology xxx (2014) xxx–xxx 7
Please cite this article in press as: Roder Green, A.L., et al. Littered cigarette butts as a source of nicotine in urban waters. J. Hydrol. (2014), http://dx.doi.org/
10.1016/j.jhydrol.2014.05.046
amounts. Furthermore, contradictory results suggest that the effect
of ashtrays on cigarette littering rates is not clear (Schultz et al.,
2013, Bator et al., 2011; Patel et al., 2013). Nevertheless, intensified
street sweeping efforts and the installation of additional ash trays
will be an economic hurdle for cities or tobacco companies
(Novotny and Zhao, 1999), with unclear effects.
Instead, we recommend a public education approach aimed at
effecting a change in littering behavior through awareness-raising.
People who consider cigarette butts to be litter are significantly
more likely to dispose of their butts properly (Rath et al., 2012).
The main message of such a campaign should focus on the toxic
nature of cigarette butt waste and the effect on environment and
drinking water quality.
Additionally, the pathways of nicotine released from cigarette
butts to urban waters are in need of investigation. We recommend
the implementation of a monitoring system for nicotine in urban
waters (surface, ground- and drinking waters). Furthermore, stud-
ies are necessary to observe nicotine not only in surface run-off but
for all pathways and transformations it may undergo at natural,
technical and natural–technical interfaces such as soil, pavement,
sewer, surface water body or WWTP and then surface water, bank
filtration, infiltration into groundwater, groundwater extraction,
drinking water treatment, drinking water, bottled water (Gessner
et al., 2014).
Acknowledgements
The authors would like to thank Prof. Gerd Wessolek, head of
the chair of soil conservation and Prof. Martin Jekel, head of the
chair of water quality control, both from the Technische Universi-
taet Berlin for their moral, financial, and infrastructural support.
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10.1016/j.jhydrol.2014.05.046
