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Development strategies for gas converting bioprocesses -CO 2 utilisation in CELBICON and ENGICOIN

Authors:
  • Krajete GmbH

Abstract

The CO2-BMP process uses selected archaea microorganisms as biological catalyst to perform a carbon activation and methanation autocatalytic reaction which converts hydrogen and carbon dioxide directly into methane, water and biomass in continuous or intermittent operations. The integrated modular development workflow consists of studying the biomethanation process from different angles and using different “levels” of pressurized H2 and CO2.The following aspects have been investigated in CELBICON project: pressure tolerance, media demands, feed strategy development for fermentation and validation runs in continuous culture to reach performances above 20 kgCH4 m-3 h-1 (MER > 1250 mmolCH4 Lbroth-1 h-1) in steady state production in order to support process simulation and tecno-economic assessment. Furthermore, the methodologies from the CO2-BMP process development are transferable to other gas converting bioprocess endeavour like performing acetone production from H2 and CO2 as in ENGICOIN project
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 1
Development strategies for gas converting
bioprocesses CO2utilisation in CELBICON and
ENGICOIN
Arne H. Seifert & Sébastien Bernacchi
CO2OLING THE EARTH, Amsterdam, 06.09.2019
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 2
Company Facts
Krajete GmbH is an Austrian company
established since 2012 and working in
three different business segments:
Biomethanation (CO2-BMP
process)
Adsorptive gas purification
Industrial gas sampling
1 granted patent & 7 patent applications
> 15 peer reviewed publications
(2011-2019) support the licensing and
tech-transfer of the proprietary
biomethanation process
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 3
“Photosynthetic Bypass”
4th generation biofuel
(> 20 kg/m3*h)
Axenic CO2-BMP process ?
A single strain process converting hydrogen and carbon dioxide to
methane, water and biomass in a defined “gassed mineral water”
[1] Sébastien Bernacchi, Christoph Herwig: “Application of a modular and interdisciplinary approach to the development of a biological methane
production (BMP) process,” 2015.
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 4
Selectivity in CO2-BMP process
Chemistry:
Need high purity feedstocks
Produces side products
Purification
Biology:
Extract nutrients from gas
mixtures
Tolerates contaminants
Stable selectivity
Biology makes from mixtures 1 product while
Chemistry makes from pure components mixtures !
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 5
CO2-BMP = CO2utilization for
CH4production!
How will the energy
transition look like?
@Sovakool et al. & Amrouche et al. & @Fossil Fuels and Emissions Forecast To Continue To Rise BP Energy Outlook
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 6
Applications for CO2-BMP?
Industry
Application
1.
Communities
Decentralized Energy Supply
by storing renewable electricity as
gas for:
a) Mobility (mechanical energy)
b) Power (electrical energy)
c) Heat (thermal energy)
2. Mobility
C Neutral Fuel
, “4th Generation Biofuels” compatible with current
combustion engines
but sustainable (e.g. automobile)
3. Power Supply
Storage of Renewables
(e.g. Power to Gas “PtG”)
4. Biogas
Direct
biogenic upgrade of Biogas to Natural Gas
5. Chemical, Steel
etc.
Direct valorization of
“waste gas” streams from anthropogenic
origins containing CO
2and/or H2to “Green” Methane
We adapt the CO2-BMP autobiocalytic process to our
client´s process declinations and integration concepts
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 7
CO2-BMP for biogas upgrade
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 8
CO2-BMP in a “PtG” frame
42 L
Pilot Reactor
Waste Incineration
Mobile Application
1 Nm3CO2/h
Ca. 4 Nm3H2/h
(via electrolyzer ran with
renewable intermittent electricity)
0.94 - 0.97 Nm3CH4/h
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 9
CO2-BMP in biorefinery frames
Coupling multiple waste streams for process intensification [2]
[2] S. BERNACCHI, B. LORANTFY, E. MARTINEZ, and C. HERWIG, “RESTRUCTURING RENEWABLE ENERGY SOURCES FOR MORE EFFICIENT BIOFUELS PRODUCTION WITH EXTREMOPHILIC
MICROORGANISMS.”; 13th Symposium Energy innovation, 12.-14.2.2014, Graz/Austria
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 10
CO2-BMP from pyrolysis gas
Gez.: N.N.
Datum: 24.10.15
METHANOGENESE - Blockfließbild
Z.Nr.: AK 009/2015
STATUS: 27.10.2015
Kerosin
Kerosin
beladen
Abwasser
Fackelgas
(Regeneration)
Fackelgas
(Regeneration)
Spülgas
Fackelgas
Inertgas
(Kamin)
Sauerstoff
GASWÄSCHE
PYROLYSEGAS
Sprühwäscher
GASTRENNUNG
Druckwechselanlage
(4 Stück)
P ~ 1 [bara]
V ~ 25 [Nm³/h]
T ~ 20 [°C]
P ~ 22 [bar]
V ~2,3 [m³/h]
T ~ 10 [°C]
VOR-
ADSORPTION
Festbettadsorber
(2 Stück)
N2CO CH4/CO2
Drucklagertank
(4 Stück)
H2
VERBRENNUNG
Klärschlamm
Sprühwäscher
Kondensat
Gasbrenner
P ~ 2 [bar]
V ~ 3,0 [m³/h]
T ~ 20 [°C]
P ~22 [bar]
V ~ 0,4 [m³/h]
T ~ 20 [°C]
P ~ 10 [bar]
V ~ 0,4 [m³/h]
T ~ 20 [°C]
ALKALISCHE
GASWÄSCHE
METHANO-
GENESE
GAS-
FEINREINIGUNG
VERKAUFSGAS
ABWASSER-
BEHANDLUNG
Flockungs-
mittel
Abwasser
Füllkörper-
wäscher
NaOH (20 %)
Rührkessel/Schräg-
lammellenklärer
Rührkessel
(5 bar)
Festbettadsorber
Abwasser
3-stufig
P ~ 22 [bar]
V ~2,3 [m³/h]
T ~ 10 [°C]
ca. 0,4 [kg/h]
P ~ 16 [bar]
V ~ 0,2 [m³/h]
T ~ 20 [°C]
ca. 1,2 [Nm³/h]
P ~5 [bar]
V ~ 1,9 [m³/h]
T ~ 20 [°C]
P ~ 5 [bar]
V ~ 0,8 [m³/h]
T ~ 20 [°C]
P ~ 5 [bar]
V ~ 0,7 [m³/h]
T ~ 20 [°C]
P ~ 5 [bar]
V ~ 1,2 [m³/h]
T ~ 20 [°C]
P ~ 4,7 [kW]
Kamin
Warmwasser H ~ 13 [kW]
P ~5 [bar]
V ~ 1,9 [m³/h]
T ~ 20 [°C]
P ~ 5 [bar]
V ~ 1,2 [m³/h]
T ~ 20 [°C]
P ~ 5 [bar]
V ~ 0,05 [m³/h]
T ~ 20 [°C]
2-stufig
P ~ 5 [bar]
V ~ 0,7 [m³/h]
T ~ 20 [°C]
P ~ 0,25 [kW]
N-Quelle
S-Quelle
P-Quelle
P ~ 1 [bar]
V ~ 3,85 [m³/h]
T ~ 20 [°C]
P ~ 1,2 [bar]
V ~ 3,4 [Nm³/h]
T ~ 60 [°C]
Kondensat
nicht im Lieferumfang
P ~ 2 [bar]
V ~ 1,7 [m³/h]
T ~ 20 [°C]
V ~ 3,0 [Nm³/h]
T ~ 20 [°C]
P ~ 2 [bar]
V ~ 3,0 [Nm³/h]
T ~ 20 [°C] Fackelgas
Luft
P ~ 1 [bar]
V ~ 3,9 [m³/h]
T ~ 20 [°C]
5 step Process
1. Condensation
2. Adsorptive separation
3. CO oxidation
4. Methanogenesis
5. Product Gas Purification
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 11
CO2-BMP & grid independency?
H2
CO2
Bio fertilizer
CH4
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 12
What do we do and how?
CO2-BMP process licensing
Feasibility studies, basic engineering and custom adaptation of the
process to client specific industrial systems
Technology transfer and support for the overall hardware system
engineering, design and construction
Customizable control based on proprietary feed strategy
Ongoing operational support and process optimization
Experimental gas transfer measurement in laminar and turbulent
operational regimes of industrial reactors
Consulting for development of new gas converting bioprocesses
Partnership for industrial and academic projects
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 13
Challenges in gas converting
bioprocess development
For further info: sebastien@krajete.com
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 14
Extremophiles ?
An extremophile is an organism that thrives in physically or
geochemically extreme conditions that are detrimental to most life
on Earth
So, HOW using extremophiles?
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 15
CO2-BMP proc. development
How should the development steps of a gas converting bioprocess
be structured?[3]
How and which key physiologic parameters need to be determined?
Which are the most important parameters for scale up? [4]
On which parameters should the bioprocess control be based?
[3] Sébastien Bernacchi, Christoph Herwig: “Application of a modular and interdisciplinary
approach to the development of a biological methane production (BMP) process,” 2015.
[4] Sébastien Bernacchi and Christoph Herwig, “Challenges and solutions for development
of gas limited bioprocesses illustrated by the biological methane production (BMP) process
development.
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 16
CO2-BMP development setups
Two “twin” bioreactor setups were used in the first 5 years of the
CO2-BMP process development
Working Volume = 5 - 10L
Working Volume = 0.5 - 1L
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 17
CO2-BMP dev. challenge
Anaerobic & continuous autobiocatalytic operation
Cultivation in a defined mineral media
Fast kinetic for M. marburgensis: qCH4,max > 115 [mmol g-1h-1]
If the biology is properly controlled, the kinetic determining step is
H2transfer rate to the liquid phase
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 18
Screening CO2-BMP process
Nona-variate screening strategy in a 3 level fractional factorial
Design of Experiment (DoE)[5,6]
Media simplification + control of the reaction selectivity
[5] S. Bernacchi, S. Rittmann, A. H. Seifert, A. Krajete, C. Herwig; “Experimental methods
for screening parameters influencing the growth to product yield (Y(x/CH4)) of a
biological methane production (BMP) process performed with Methanothermobacter
marburgensis,” AIMS Bioeng., vol. 1, no. 2, pp. 7286, 2014.
[6] Krajete GmbH patent application: “Method and system for producing methane using
methanogenic microorganisms and applying specific nitrogen concentrations in the
liquid phase.”
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 19
CO2-BMP & PATs
Balancing on molar basis (C-mol, N-mol, S-mol etc..)
E.g. C-balance: CO2,in =CO2,out +CH4,out +HCO3-out + Cbiomass,out
Gaseous compounds and main nutrients quantified in ppm range and
trace elements up to ppb for quantification of scalable uptake rates [7]
[7] W. Nischkauer, F. Vanhaecke, S. Bernacchi, C. Herwig, and A. Limbeck, “Radial line-scans as representative sampling strategy in dried-droplet
laser ablation of liquid samples deposited on pre-cut filter paper disks,” Spectrochim. Acta Part B At. Spectrosc., vol. 101, pp. 123129, Nov. 2014.
ICP-OES/MS
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 20
CO2-BMP & intermittency
A challenging offgas
quantification:
Stable for monitoring
Fast for resolution of
dynamic profiles
Reliable for direct offgas
measurement
Accurate for multiple
components: H2, N2, O2,
CO, CO2, CH4
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 21
CO2-BMP & real gas sources
Our industrial gas sampling service was developed to evaluate in-
house our bioprocess tolerance to real impurities that are contained in
real industrial gases such as raw biogas, combustion gas or syngas [8]
Type of Gas Convertable component Concentration [Vol.-%] Other components
Synthetic H2 enriched waste gas H2 ~60 CO,CO2, short-chain alkanes
Impure biogas CO2 ~50 CH4, unknown
Combustion gas CO2 ~10 mainly N2, O2
Experiment Nr°
Experiment type Real gas Reference Real gas Reference Real gas Reference
Total flow rate [vvm] 0.54 0.501 0.625
Flow rate H2 [NL/min] 0 1.527 1.625 1.625 0.2224 0.2224
Flow rate CO2 [NL/min] 0.3 0.348 0 0.4048 0.0276 0.0556
Flow rate real gas/N2 [NL/min] 2.424 0.848 0.88 0.4752 0.25 0.222
Real gas content [Vol.-%] 89 - 35.1 - 50 -
Reactor volume [L]
Reactor pressure [barg]
MERReal / MERRef
Combustion gas
5
0.8
1.07 ± 0.076
1.07 ± 0.12
0
0
1
3
Synthetic H2-enriched waste gas
[8] A. H. Seifert, S. Rittmann, S. Bernacchi, and C. Herwig, “Method for assessing the impact of emission gasses on physiology and productivity in
biological methanogenesis,” Bioresour. Technol., vol. 136, pp. 747751, May 2013.
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 22
CO2-BMPin silico” process
Use a process simulation environment to assess the CO2-BMP process
efficiency in a power to gas frame to perform easy sensitivity analysis
on KPP for sustaining scale up and process design activities [9]
Calculation of G/L equilibrium to cross validate balancing results
[9] S. Bernacchi, M. Weissgram, W. Wukovits, C. Herwig; “Process efficiency simulation for key process parameters in biological
methanogenesis,” AIMS Bioeng., vol. 1, no. 1, pp. 5371, 2014.
Is pressure
tolerated?
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 23
CO2-BMP & high pressure
In order to enhance the gas transfer rate [10]of hydrogen to the liquid
phase, the use of pressure was investigated
Tech-transfer of a simplified CO2-BMP setup for liquid fed-batch and
continuously gassed experiments at 10 barg implemented at JKU (Linz)
[10] A.H. Seifert, S. Rittmann, C. Herwig, Analysis of process related factors to increase volumetric productivity and quality of biomethane with
Methanothermobacter marburgensis, Applied Energy, Volume 132, 2014, Pages 155-162
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 24
CO2-BMP scale up test setup
450 L“traditional” vessel with a bit of “customization” to assess the
process performance in bigger volumes while using “bulky”
substrate(s) and investigating the reaction exothermicity
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 25
CO2-BMP control strategy
Development of a patented feed forward
model based control strategy for
automation + enhanced performance [11]
b
[11] S. Bernacchi, A. Krajete, C. Herwig; “Experimental workflow for developing a feed forward strategy to control biomass growth and
exploit maximum specific methane productivity of Methanothermobacter marburgensis in a biological methane production process (BMPP),”
AIMS Microbiol., vol. 2, no. 3, pp. 262277, 2016.
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 26
H2020 Celbicon project
WP 6 leader for TP2 engineering, design and assembly
www.Celbicon.org PFD
P&I D
Hazards Identified S x L (Before Risk Reduction)
Hazards Identified S x L (After Risk Reduction)
HAZOP
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 27
Celbicon development workflow
Temperature & strain screening: Test the growth attribute of mesophilic, thermophilic and
hyperthermophilic methanogenic archaea strains up to 3bar in closed batch glass vessels. Use of
referenced media from strain banks and then simplification of media in a second screening step to
use only defined mineral media without addition of complex substrates.
High pressure screening: Determine the intrinsic capacity of a given strain to cope with
pressurization and depressurization in a defined mineral media without addition of complex
substrates and support long term exposure to pressure of at least 10 [barg] .
Media development: Aims to develop a media composition able to maintain enough biomass
and correlated biocatalytic activity to assess the strain specific methane productivity (qCH4given in
[mmolCH4/(g*h)]) and determine more precisely how growth is affected by process parameters
such as temperature, pH, agitation, shear stress or gassing rate.
Feed development: development of a feeding strategy to maintain biologic methane production
in continuous operations in order to quantify nutrient requirements in real operation scenarios
Validation runs selected microorganisms and development of an advanced feed strategy
enabling the process to reach a stable performance at methane productivities >20 [kgCH4/m3*h]
(MER = 1250 [mmolCH4/L*h]) with >95 Vol% CH4contained in the raw wet gas
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 28
CO2-BMP strain screening
>80 methanogenic
(mesophilic, thermophilic &
hyperthermophilic) strains
screened at low and high
pressure
High pressure screening
setup used to investigate
methanogens physiology
while mimicking extra-
terrestrial conditions [12]
[12] R.-S. Taubner et al., “Biological methane production under putative Enceladus-like conditions,” Nat. Commun., vol. 9, no. 1, Dec. 2018.
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 29
CO2-BMP kinetic aspects
PCA on a 18 parameters sub-dataset consisting of gas limited st-st
Round surface modelling performed for qCH4 and MER “responses”
with 4 input var.: Dilution rate, temperature, agitation and gassing[13]
[13] S. K.-M. R. Rittmann, A. H. Seifert, and S. Bernacchi, “Kinetics, multivariate statistical modelling, and physiology of CO 2 -based biological methane
production,” Appl. Energy, vol. 216, pp. 751760, Apr. 2018.
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 30
CO2-BMP - R&D facility
The “mother” reactor for further development of CO2-BMP at
pressure up to 15 barg at MER = 1500 (ca. 33 Nm3mr-3 h-1)
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 31
H2020 - ENGICOIN
CO2-BMP process know-how is used for other gas converting
bioprocess development at elevated pressure: www.Engicoin.eu
From lab scale data to development of a TRL 5 bioprocess in a 200 L pilot
Our role consist of WP management, elaboration of DoEs, data treatment to feed modelling and
process simulation activities as well as supporting engineering and process design
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 32
ENGICOIN development workflow
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 33
From In vivo to in silico
Combination of dynamic and chemostat experiments to quantify
scalable molar based KPP on the upstream process
Elaboration of growth and product kinetic models to translate
experimental data into mode for various in silico environments
Use of upstream process models to design, engineer and optimize the
downstream process for acetone recovery
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 34
Questions ?
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 35
Thank you for your attention !
eMail: info@krajete.com Web: www.krajete.com
Krajete GmbH 36
References
[1] Sébastien Bernacchi, Christoph Herwig: “Application of a modular and interdisciplinary approach to the
development of a biological methane production (BMP) process,” 2015.
[2] S. BERNACCHI, B. LORANTFY, E. MARTINEZ, and C. HERWIG, “RESTRUCTURING RENEWABLE ENERGY SOURCES FOR
MORE EFFICIENT BIOFUELS PRODUCTION WITH EXTREMOPHILIC MICROORGANISMS.;13th Symposium Energy
innovation, 12.-14.2.2014, Graz/Austria
[3] S. Bernacchi, Christoph Herwig: “Application of a modular and interdisciplinary approach to the development of a
biological methane production (BMP) process,2015.
[4] S. Bernacchi and Christoph Herwig, “Challenges and solutions for development of gas limited bioprocesses
illustrated by the biological methane production (BMP) process development.
[5] S. Bernacchi, S. Rittmann, A. H. Seifert, A. Krajete, C. Herwig; “Experimental methods for screening parameters
influencing the growth to product yield (Y(x/CH4)) of a biological methane production (BMP) process performed with
Methanothermobacter marburgensis,AIMS Bioeng., vol. 1, no. 2, pp.7286,2014.
[6] Krajete GmbH patent application:“Method and system for producing methane using methanogenic
microorganisms and applying specific nitrogen concentrations in the liquid phase.
[7] W. Nischkauer, F. Vanhaecke, S. Bernacchi, C. Herwig, and A. Limbeck, “Radial line-scans as representative
sampling strategy in dried-droplet laser ablation of liquid samples deposited on pre-cut filter paper disks,”
Spectrochim. Acta Part B At. Spectrosc., vol. 101,pp.123129, Nov. 2014
[8] A. H. Seifert, S. Rittmann, S. Bernacchi, and C. Herwig, “Method for assessing the impact of emission gasses on
physiology and productivity in biological methanogenesis,Bioresour. Technol., vol. 136,pp.747751, May 2013.
[9] S. Bernacchi, M. Weissgram, W. Wukovits, C. Herwig; “Process efficiency simulation for key process parameters in
biological methanogenesis,AIMS Bioeng., vol. 1, no. 1, pp.5371,2014.
[10]A.H. Seifert, S. Rittmann, C. Herwig, Analysis of process related factors to increase volumetric productivity and
quality of biomethane with Methanothermobacter marburgensis, Applied Energy, Volume 132,2014, Pages 155-162
[11]S. Bernacchi, A. Krajete, C. Herwig; “Experimental workflow for developing a feed forward strategy to control
biomass growth and exploit maximum specific methane productivity of Methanothermobacter marburgensis in a
biological methane production process (BMPP),AIMS Microbiol., vol. 2, no. 3, pp.262277,2016.
[12] R.-S. Taubner et al., “Biological methane production under putative Enceladus-like conditions,” Nat. Commun.,
vol. 9, no. 1, Dec. 2018
[13] S. K.-M. R. Rittmann, A. H. Seifert, and S. Bernacchi,“Kinetics, multivariate statistical modelling, and physiology
of CO 2 -based biological methane production,” Appl. Energy, vol. 216,pp.751760, Apr. 2018.
... During laboratory scale tests (at 15 bars), Krajete obtained interesting results with productivities reaching 33 m 3 CH 4 /m 3 reactor/h. Further tests were undertaken in a "customized" 450 L reactor in order to assess the performance of the process in larger volumes [101]. However, to our knowledge, no results from these tests are available to date. ...
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