Integrated Capture and Conversion of CO2 to Methane Using a Water-lean, Post-Combustion CO2 Capture Solvent

Kothandaraman, Jotheeswari; Saavedra Lopez, Johnny; Jiang, Yuan; Walter, Eric D.; Burton, Sarah D.; Dagle, Robert A.; Heldebrant, David J.

doi:10.1002/cssc.202101590

Title: Integrated Capture and Conversion of CO₂ to Methane Using a Water-lean, Post-Combustion CO₂ Capture Solvent

Journal Article · 20 August 2021 · ChemSusChem

DOI: https://doi.org/10.1002/cssc.202101590 · OSTI ID:1829683

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Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Integrated Carbon Capture and Conversion of CO₂ into materials (IC3M) is an attractive solution to meet the global energy demand, reduce our dependence on fossil fuels and lower CO₂ emissions. In this work, using a water-lean post combustion capture solvent, (N-(2-ethoxyethyl)-3-morpholinopropan-1-amine) (2-EEMPA), >90% conversion of captured CO2 to hydrocarbons, mostly methane, is achieved in the presence of a heterogenous Ru catalysts under relatively mild reaction conditions (170 °C and <15 bar H₂ pressure). The catalytic performance was better in 2-EEMPA than aqueous 5M monoethanol amine (MEA). Operando NMR study showed in-situ formation of N-formamide intermediate, which underwent further hydrogenation to form methane and other higher hydrocarbons. The technoeconomic analyses (TEA) showed that the proposed integrated process can potentially improve the thermal efficiency by 5% and reduce the total capital investment and minimum synthetic natural gas (SNG) selling price by 32% and 12% respectively compared to conventional Sabatier process, highlighting the energetic and economic benefits of integrated capture and conversion. Methane derived from CO₂ and renewable H₂ source is an attractive fuel, and it has a great potential as a renewable hydrogen carrier as an environmentally responsible carbon capture and utilization approach.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1829683

Report Number(s):: PNNL-SA--162553

Journal Information:: ChemSusChem, Journal Name: ChemSusChem Journal Issue: 21 Vol. 14; ISSN 1864-5631

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

References (58)

Selektive katalytische Synthesen mit Kohlendioxid und Wasserstoff: Katalyse-Schach an der Nahtstelle zwischen Energie und Chemie Klankermayer, Jürgen; Wesselbaum, Sebastian; Beydoun, Kassem Angewandte Chemie, Vol. 128, Issue 26 https://doi.org/10.1002/ange.201507458	journal	May 2016
Selective Catalytic Synthesis Using the Combination of Carbon Dioxide and Hydrogen: Catalytic Chess at the Interface of Energy and Chemistry Klankermayer, Jürgen; Wesselbaum, Sebastian; Beydoun, Kassem Angewandte Chemie International Edition, Vol. 55, Issue 26 https://doi.org/10.1002/anie.201507458	journal	May 2016
Are Amines the Holy Grail for Facilitating CO ₂ Reduction? Jakobsen, Joakim B.; Rønne, Magnus H.; Daasbjerg, Kim Angewandte Chemie International Edition, Vol. 60, Issue 17 https://doi.org/10.1002/anie.202014255	journal	March 2021
CO 2 Capture and Conversion with a Multifunctional Polyethyleneimine-Tethered Iminophosphine Iridium Catalyst/Adsorbent McNamara, Nicholas D.; Hicks, Jason C. ChemSusChem, Vol. 7, Issue 4 https://doi.org/10.1002/cssc.201301231	journal	March 2014
Carbon Dioxide Hydrogenation into Higher Hydrocarbons and Oxygenates: Thermodynamic and Kinetic Bounds and Progress with Heterogeneous and Homogeneous Catalysis Prieto, Gonzalo ChemSusChem, Vol. 10, Issue 6 https://doi.org/10.1002/cssc.201601591	journal	March 2017
Aqueous Biphasic Systems for the Synthesis of Formates by Catalytic CO ₂ Hydrogenation: Integrated Reaction and Catalyst Separation for CO ₂ -Scrubbing Solutions Scott, Martin; Blas Molinos, Beatriz; Westhues, Christian ChemSusChem, Vol. 10, Issue 6 https://doi.org/10.1002/cssc.201601814	journal	February 2017
Electrocatalytic Reduction of CO ₂ to Methanol by Iron Tetradentate Phosphine Complex Through Amidation Strategy Bi, Jiaojiao; Hou, Pengfei; Liu, Fang‐Wei ChemSusChem, Vol. 12, Issue 10 https://doi.org/10.1002/cssc.201802929	journal	April 2019
Molecular‐Level Overhaul of γ‐Aminopropyl Aminosilicone/Triethylene Glycol Post‐Combustion CO ₂ ‐Capture Solvents Cantu, David C.; Malhotra, Deepika; Nguyen, Manh‐Thuong ChemSusChem, Vol. 13, Issue 13 https://doi.org/10.1002/cssc.202000724	journal	June 2020
CO ₂ Reduction to Methanol in the Liquid Phase: A Review Xie, Shaoqu; Zhang, Wanli; Lan, Xingying ChemSusChem https://doi.org/10.1002/cssc.202002087	journal	November 2020
Tertiary Amine‐Ethylene Glycol Based Tandem CO ₂ Capture and Hydrogenation to Methanol: Direct Utilization of Post‐Combustion CO ₂ Sen, Raktim; Koch, Christopher J.; Goeppert, Alain ChemSusChem https://doi.org/10.1002/cssc.202002285	journal	November 2020
Strategies for Integrated Capture and Conversion of CO ₂ from Dilute Flue Gases and the Atmosphere Maina, James W.; Pringle, Jennifer M.; Razal, Joselito M. ChemSusChem, Vol. 14, Issue 8 https://doi.org/10.1002/cssc.202100010	journal	March 2021
Carbon Capture and Utilization Update Al-Mamoori, Ahmed; Krishnamurthy, Anirudh; Rownaghi, Ali A. Energy Technology, Vol. 5, Issue 6 https://doi.org/10.1002/ente.201600747	journal	March 2017
CO and CO2 methanation over Ni catalysts supported on CeO2, Al2O3 and Y2O3 oxides Italiano, C.; Llorca, J.; Pino, L. Applied Catalysis B: Environmental, Vol. 264 https://doi.org/10.1016/j.apcatb.2019.118494	journal	May 2020
Advances in carbon capture, utilization and storage Zhang, Zhien; Wang, Tao; Blunt, Martin J. Applied Energy, Vol. 278 https://doi.org/10.1016/j.apenergy.2020.115627	journal	November 2020
Global challenges and strategies for control, conversion and utilization of CO2 for sustainable development involving energy, catalysis, adsorption and chemical processing Song, Chunshan Catalysis Today, Vol. 115, Issue 1-4 https://doi.org/10.1016/j.cattod.2006.02.029	journal	June 2006
Methanation of carbon dioxide on Ru/Al2O3: Catalytic activity and infrared study Garbarino, Gabriella; Bellotti, Daria; Finocchio, Elisabetta Catalysis Today, Vol. 277 https://doi.org/10.1016/j.cattod.2015.12.010	journal	November 2016
Use of monoethanolamine (MEA) for CO 2 capture in a global scenario: Consequences and alternatives Luis, Patricia Desalination, Vol. 380 https://doi.org/10.1016/j.desal.2015.08.004	journal	February 2016
Techno-economic comparison of various process configurations for post-combustion carbon capture using a single-component water-lean solvent Jiang, Yuan; Mathias, Paul M.; Freeman, Charles J. International Journal of Greenhouse Gas Control, Vol. 106 https://doi.org/10.1016/j.ijggc.2021.103279	journal	March 2021
Chemical transformations of captured CO2 into cyclic and polymeric carbonates Kothandaraman, Jotheeswari; Zhang, Jun; Glezakou, Vassiliki-Alexandra Journal of CO2 Utilization, Vol. 32 https://doi.org/10.1016/j.jcou.2019.04.020	journal	July 2019
Tandem and Hybrid Processes for Carbon Dioxide Utilization Overa, Sean; Feric, Tony G.; Park, Ah-Hyung Alissa Joule, Vol. 5, Issue 1 https://doi.org/10.1016/j.joule.2020.12.004	journal	January 2021
Integrated CO ₂ Capture and Conversion to Formate and Methanol: Connecting Two Threads Kar, Sayan; Goeppert, Alain; Prakash, G. K. Surya Accounts of Chemical Research, Vol. 52, Issue 10 https://doi.org/10.1021/acs.accounts.9b00324	journal	September 2019
Water-Lean Solvents for Post-Combustion CO ₂ Capture: Fundamentals, Uncertainties, Opportunities, and Outlook Heldebrant, David J.; Koech, Phillip K.; Glezakou, Vassiliki-Alexandra Chemical Reviews, Vol. 117, Issue 14 https://doi.org/10.1021/acs.chemrev.6b00768	journal	May 2017
Recent Advancements, Fundamental Challenges, and Opportunities in Catalytic Methanation of CO ₂ Younas, Muhammad; Loong Kong, Leong; Bashir, Mohammed J. K. Energy & Fuels, Vol. 30, Issue 11 https://doi.org/10.1021/acs.energyfuels.6b01723	journal	October 2016
Dual-Function Materials for CO ₂ Capture and Conversion: A Review Omodolor, Ibeh S.; Otor, Hope O.; Andonegui, Joseph A. Industrial & Engineering Chemistry Research, Vol. 59, Issue 40 https://doi.org/10.1021/acs.iecr.0c02218	journal	August 2020
The Role of Carbon Capture and Utilization, Carbon Capture and Storage, and Biomass to Enable a Net-Zero-CO ₂ Emissions Chemical Industry Gabrielli, Paolo; Gazzani, Matteo; Mazzotti, Marco Industrial & Engineering Chemistry Research, Vol. 59, Issue 15 https://doi.org/10.1021/acs.iecr.9b06579	journal	March 2020
Operando MAS NMR Reaction Studies at High Temperatures and Pressures Walter, Eric D.; Qi, Long; Chamas, Ali The Journal of Physical Chemistry C, Vol. 122, Issue 15 https://doi.org/10.1021/acs.jpcc.7b11442	journal	January 2018
Recycling Carbon Dioxide through Catalytic Hydrogenation: Recent Key Developments and Perspectives Ra, Eun Cheol; Kim, Kwang Young; Kim, Eun Hyup ACS Catalysis, Vol. 10, Issue 19 https://doi.org/10.1021/acscatal.0c02930	journal	August 2020
Combining Low-Pressure CO ₂ Capture and Hydrogenation To Form Methanol Khusnutdinova, Julia R.; Garg, Jai Anand; Milstein, David ACS Catalysis, Vol. 5, Issue 4 https://doi.org/10.1021/acscatal.5b00194	journal	March 2015
Integrating CO ₂ Electrolysis into the Gas-to-Liquids–Power-to-Liquids Process van Bavel, Svetlana; Verma, Sumit; Negro, Emanuela ACS Energy Letters, Vol. 5, Issue 8 https://doi.org/10.1021/acsenergylett.0c01418	journal	July 2020
Transformation of Carbon Dioxide Sakakura, Toshiyasu; Choi, Jun-Chul; Yasuda, Hiroyuki Chemical Reviews, Vol. 107, Issue 6 https://doi.org/10.1021/cr068357u	journal	June 2007
Molecular Separation with Organic Solvent Nanofiltration: A Critical Review Marchetti, Patrizia; Jimenez Solomon, Maria F.; Szekely, Gyorgy Chemical Reviews, Vol. 114, Issue 21 https://doi.org/10.1021/cr500006j	journal	October 2014
Methanol from CO ₂ by Organo-Cocatalysis: CO ₂ Capture and Hydrogenation in One Process Step Reller, Christian; Pöge, Matthias; Lißner, Andreas Environmental Science & Technology, Vol. 48, Issue 24 https://doi.org/10.1021/es503914d	journal	November 2014
Homogeneous Hydrogenation of CO ₂ to Methyl Formate Utilizing Switchable Ionic Liquids Yadav, Mahendra; Linehan, John C.; Karkamkar, Abhijeet J. Inorganic Chemistry, Vol. 53, Issue 18 https://doi.org/10.1021/ic501378w	journal	August 2014
Anthropogenic Chemical Carbon Cycle for a Sustainable Future Olah, George A.; Prakash, G. K. Surya; Goeppert, Alain Journal of the American Chemical Society, Vol. 133, Issue 33 https://doi.org/10.1021/ja202642y	journal	August 2011
Tandem Amine and Ruthenium-Catalyzed Hydrogenation of CO ₂ to Methanol Rezayee, Nomaan M.; Huff, Chelsea A.; Sanford, Melanie S. Journal of the American Chemical Society, Vol. 137, Issue 3 https://doi.org/10.1021/ja511329m	journal	January 2015
Chemical Recycling of Carbon Dioxide to Methanol and Dimethyl Ether: From Greenhouse Gas to Renewable, Environmentally Carbon Neutral Fuels and Synthetic Hydrocarbons Olah, George A.; Goeppert, Alain; Prakash, G. K. Surya The Journal of Organic Chemistry, Vol. 74, Issue 2, p. 487-498 https://doi.org/10.1021/jo801260f	journal	January 2009
Using carbon dioxide as a building block in organic synthesis Liu, Qiang; Wu, Lipeng; Jackstell, Ralf Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms6933	journal	January 2015
CO2 hydrogenation to high-value products via heterogeneous catalysis Ye, Run-Ping; Ding, Jie; Gong, Weibo Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-13638-9	journal	December 2019
Electrochemical upgrade of CO2 from amine capture solution Lee, Geonhui; Li, Yuguang C.; Kim, Ji-Yong Nature Energy, Vol. 6, Issue 1 https://doi.org/10.1038/s41560-020-00735-z	journal	December 2020
The technological and economic prospects for CO2 utilization and removal Hepburn, Cameron; Adlen, Ella; Beddington, John Nature, Vol. 575, Issue 7781 https://doi.org/10.1038/s41586-019-1681-6	journal	November 2019
Catalysis mechanisms of CO ₂ and CO methanation Miao, Bin; Ma, Su Su Khine; Wang, Xin Catalysis Science & Technology, Vol. 6, Issue 12 https://doi.org/10.1039/C6CY00478D	journal	January 2016
CO ₂ capture by amines in aqueous media and its subsequent conversion to formate with reusable ruthenium and iron catalysts Kothandaraman, Jotheeswari; Goeppert, Alain; Czaun, Miklos Green Chemistry, Vol. 18, Issue 21 https://doi.org/10.1039/C6GC01165A	journal	January 2016
The steps of activating a prospective CO ₂ hydrogenation catalyst with combined CO ₂ capture and reduction Lao, D. B.; Galan, B. R.; Linehan, J. C. Green Chemistry, Vol. 18, Issue 18 https://doi.org/10.1039/C6GC01800A	journal	January 2016
Life cycle assessment of CO ₂ -based C1-chemicals Sternberg, André; Jens, Christian M.; Bardow, André Green Chemistry, Vol. 19, Issue 9 https://doi.org/10.1039/C6GC02852G	journal	January 2017
Carbon capture and storage (CCS): the way forward Bui, Mai; Adjiman, Claire S.; Bardow, André Energy & Environmental Science, Vol. 11, Issue 5 https://doi.org/10.1039/C7EE02342A	journal	January 2018
A short review of recent advances in CO 2 hydrogenation to hydrocarbons over heterogeneous catalysts Li, Wenhui; Wang, Haozhi; Jiang, Xiao RSC Advances, Vol. 8, Issue 14 https://doi.org/10.1039/C7RA13546G	journal	January 2018
Condensed-phase low temperature heterogeneous hydrogenation of CO ₂ to methanol Kothandaraman, Jotheeswari; Dagle, Robert A.; Dagle, Vanessa Labarbier Catalysis Science & Technology, Vol. 8, Issue 19 https://doi.org/10.1039/C8CY00997J	journal	January 2018
Renewable energy storage via efficient reversible hydrogenation of piperidine captured CO 2 Lu, Mi; Zhang, Jianghao; Yao, Yao Green Chemistry, Vol. 20, Issue 18 https://doi.org/10.1039/C8GC00954F	journal	January 2018
A call to (green) arms: a rallying cry for green chemistry and engineering for CO ₂ capture, utilisation and storage Leclaire, Julien; Heldebrant, David J. Green Chemistry, Vol. 20, Issue 22 https://doi.org/10.1039/C8GC01962B	journal	January 2018
Methylformate from CO 2 : an integrated process combining catalytic hydrogenation and reactive distillation Scott, Martin; Westhues, Christian G.; Kaiser, Teresa Green Chemistry, Vol. 21, Issue 23 https://doi.org/10.1039/C9GC03006A	journal	January 2019
Towards environmentally benign capture and conversion: heterogeneous metal catalyzed CO ₂ hydrogenation in CO ₂ capture solvents Kothandaraman, Jotheeswari; Heldebrant, David J. Green Chemistry, Vol. 22, Issue 3 https://doi.org/10.1039/C9GC03449H	journal	January 2020
A single-component water-lean post-combustion CO ₂ capture solvent with exceptionally low operational heat and total costs of capture – comprehensive experimental and theoretical evaluation Zheng, Richard F.; Barpaga, Dushyant; Mathias, Paul M. Energy & Environmental Science, Vol. 13, Issue 11 https://doi.org/10.1039/D0EE02585B	journal	January 2020
Catalytic coproduction of methanol and glycol in one pot from epoxide, CO ₂ , and H ₂ Kothandaraman, Jotheeswari; Heldebrant, David J. RSC Advances, Vol. 10, Issue 69 https://doi.org/10.1039/D0RA09459E	journal	January 2020
A thermodynamic analysis of methanation reactions of carbon oxides for the production of synthetic natural gas Gao, Jiajian; Wang, Yingli; Ping, Yuan RSC Advances, Vol. 2, Issue 6 https://doi.org/10.1039/c2ra00632d	journal	January 2012
Carbon dioxide hydrogenation over nickel-, ruthenium-, and copper-based catalysts: Review of kinetics and mechanism Jalama, Kalala Catalysis Reviews, Vol. 59, Issue 2 https://doi.org/10.1080/01614940.2017.1316172	journal	April 2017
Separation of CO ₂ from Flue Gas: A Review Aaron, Douglas; Tsouris, Costas Separation Science and Technology, Vol. 40, Issue 1-3 https://doi.org/10.1081/SS-200042244	journal	January 2005
Production of Synthetic Natural Gas From Carbon Dioxide and Renewably Generated Hydrogen: A Techno-Economic Analysis of a Power-to-Gas Strategy Becker, William L.; Penev, Michael; Braun, Robert J. Journal of Energy Resources Technology, Vol. 141, Issue 2 https://doi.org/10.1115/1.4041381	journal	September 2018
Love at second sight for CO2 and H2 in organic synthesis Klankermayer, J.; Leitner, W. Science, Vol. 350, Issue 6261 https://doi.org/10.1126/science.aac7997	journal	November 2015

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