The effect of catholyte and catalyst layer binders on CO2 electroreduction selectivity

Chen, Yingying; Wrubel, Jacob A.; Vise, Ashlee E.; Intia, Fry; Harshberger, Samantha; Klein, Ellis; Smith, Wilson A.; Ma, Zhiwen; Deutsch, Todd G.; Neyerlin, Kenneth C.

doi:10.1016/j.checat.2022.01.011

The effect of catholyte and catalyst layer binders on CO₂ electroreduction selectivity

Journal Article · Tue Feb 08 04:00:00 EST 2022 · Chem Catalysis

DOI:https://doi.org/10.1016/j.checat.2022.01.011· OSTI ID:1860233

^[1]; ^[1]; ^[1]; Intia, Fry ^[1]; Harshberger, Samantha ^[2]; Klein, Ellis ^[1]; Smith, Wilson A. ^[3]; ^[1]; ^[1]; Neyerlin, Kenneth C. ^[1]

National Renewable Energy Lab. (NREL), Golden, CO (United States)
Fort Range Community College, Westminster, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)

Electrochemical reduction of carbon dioxide (CO₂) is an attractive technology for converting CO₂ to value-added chemicals by using renewably generated electricity. This work combines both experimental and theoretical analyses to investigate the role of different catalysts (Ag/Vu and SnO₂/Vu), binder materials, and catholyte compositions on the selectivity of a CO₂ electrolysis cell to the two-electron CO₂ reduction products CO and formate. As a complementary effort, a 2D multi-physics transport model was developed to elucidate the fundamental processes and species concentrations in the cathode components. It was shown that the selectivity of CO₂ reduction to CO can change significantly when different catholyte compositions and binder materials are used, whereas the selectivity of CO₂ to formate is relatively stable across the conditions studied. These insights can be used to inform decisions regarding the electrode development and system design in CO₂ electrolyzers and ultimately contribute to scaling energy-efficient electrochemical CO₂-reduction systems.

View Accepted Manuscript (DOE)

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Hydrogen and Fuel Cell Technologies Office (EE-3F)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1860233

Report Number(s):: NREL/JA-5700-79956; MainId:40163; UUID:de8a839a-db76-4c83-b599-2329e3674c80; MainAdminID:63315

Journal Information:: Chem Catalysis, Journal Name: Chem Catalysis Journal Issue: 2 Vol. 2; ISSN 2667-1093

Publisher:: Cell PressCopyright Statement

Country of Publication:: United States

Language:: English

References (51)

Understanding the Role of Functional Groups in Polymeric Binder for Electrochemical Carbon Dioxide Reduction on Gold Nanoparticles Lee, Ji Hoon; Kattel, Shyam; Xie, Zhenhua Advanced Functional Materials, Vol. 28, Issue 45 https://doi.org/10.1002/adfm.201804762	journal	September 2018
Electrochemical CO ₂ Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design Kibria, Md Golam; Edwards, Jonathan P.; Gabardo, Christine M. Advanced Materials, Vol. 31, Issue 31 https://doi.org/10.1002/adma.201807166	journal	December 2018
Calculation for the cathode surface concentrations in the electrochemical reduction of CO2 in KHCO3 solutions Gupta, N.; Gattrell, M.; MacDougall, B. Journal of Applied Electrochemistry, Vol. 36, Issue 2 https://doi.org/10.1007/s10800-005-9058-y	journal	October 2005
Stable surface oxygen on nanostructured silver for efficient CO2 electroreduction Jee, Michael Shincheon; Kim, Haeri; Jeon, Hyo Sang Catalysis Today, Vol. 288 https://doi.org/10.1016/j.cattod.2016.09.026	journal	June 2017
Progress toward Commercial Application of Electrochemical Carbon Dioxide Reduction Chen, Chi; Khosrowabadi Kotyk, Juliet F.; Sheehan, Stafford W. Chem, Vol. 4, Issue 11 https://doi.org/10.1016/j.chempr.2018.08.019	journal	November 2018
Electrochemical reduction of SnO2 to Sn from the Bottom: In-Situ formation of SnO2/Sn heterostructure for highly efficient electrochemical reduction of carbon dioxide to formate Ning, Shunlian; Wang, Jigang; Xiang, Dong Journal of Catalysis, Vol. 399 https://doi.org/10.1016/j.jcat.2021.04.028	journal	July 2021
Electrolytic Conversion of Bicarbonate into CO in a Flow Cell Li, Tengfei; Lees, Eric W.; Goldman, Maxwell Joule, Vol. 3, Issue 6 https://doi.org/10.1016/j.joule.2019.05.021	journal	June 2019
Enhanced performance of gas diffusion electrode for electrochemical reduction of carbon dioxide to formate by adding polytetrafluoroethylene into catalyst layer Wang, Qinian; Dong, Heng; Yu, Han Journal of Power Sources, Vol. 279 https://doi.org/10.1016/j.jpowsour.2014.12.118	journal	April 2015
Tailoring electrode microstructure via ink content to enable improved rated power performance for platinum cobalt/high surface area carbon based polymer electrolyte fuel cells Van Cleve, Tim; Wang, Guanxiong; Mooney, Mason Journal of Power Sources, Vol. 482 https://doi.org/10.1016/j.jpowsour.2020.228889	journal	January 2021
Electrochemical CO2 reduction: Electrocatalyst, reaction mechanism, and process engineering Lu, Qi; Jiao, Feng Nano Energy, Vol. 29 https://doi.org/10.1016/j.nanoen.2016.04.009	journal	November 2016
Highly selective and scalable CO2 to CO - Electrolysis using coral-nanostructured Ag catalysts in zero-gap configuration Lee, Woong Hee; Ko, Young-Jin; Choi, Yongjun Nano Energy, Vol. 76 https://doi.org/10.1016/j.nanoen.2020.105030	journal	October 2020
Progress and Perspectives of Electrochemical CO ₂ Reduction on Copper in Aqueous Electrolyte Nitopi, Stephanie; Bertheussen, Erlend; Scott, Soren B. Chemical Reviews, Vol. 119, Issue 12 https://doi.org/10.1021/acs.chemrev.8b00705	journal	April 2019
General Techno-Economic Analysis of CO ₂ Electrolysis Systems Jouny, Matthew; Luc, Wesley; Jiao, Feng Industrial & Engineering Chemistry Research, Vol. 57, Issue 6 https://doi.org/10.1021/acs.iecr.7b03514	journal	February 2018
Preferentially Oriented Ag Nanocrystals with Extremely High Activity and Faradaic Efficiency for CO ₂ Electrochemical Reduction to CO Peng, Xiong; Karakalos, Stavros G.; Mustain, William E. ACS Applied Materials & Interfaces, Vol. 10, Issue 2 https://doi.org/10.1021/acsami.7b16164	journal	January 2018
Dictating Pt-Based Electrocatalyst Performance in Polymer Electrolyte Fuel Cells, from Formulation to Application Van Cleve, Tim; Khandavalli, Sunilkumar; Chowdhury, Anamika ACS Applied Materials & Interfaces, Vol. 11, Issue 50 https://doi.org/10.1021/acsami.9b17614	journal	November 2019
Understanding Selectivity for the Electrochemical Reduction of Carbon Dioxide to Formic Acid and Carbon Monoxide on Metal Electrodes Feaster, Jeremy T.; Shi, Chuan; Cave, Etosha R. ACS Catalysis, Vol. 7, Issue 7 https://doi.org/10.1021/acscatal.7b00687	journal	June 2017
Kinetic Analysis on the Role of Bicarbonate in Carbon Dioxide Electroreduction at Immobilized Cobalt Phthalocyanine Zeng, Joy S.; Corbin, Nathan; Williams, Kindle ACS Catalysis, Vol. 10, Issue 7 https://doi.org/10.1021/acscatal.9b05272	journal	March 2020
Modifying the Electrocatalyst–Ionomer Interface via Sulfonated Poly(ionic liquid) Block Copolymers to Enable High-Performance Polymer Electrolyte Fuel Cells Li, Yawei; Van Cleve, Tim; Sun, Rui ACS Energy Letters, Vol. 5, Issue 6 https://doi.org/10.1021/acsenergylett.0c00532	journal	April 2020
A Robust, Scalable Platform for the Electrochemical Conversion of CO ₂ to Formate: Identifying Pathways to Higher Energy Efficiencies Chen, Yingying; Vise, Ashlee; Klein, W. Ellis ACS Energy Letters, Vol. 5, Issue 6 https://doi.org/10.1021/acsenergylett.0c00860	journal	May 2020
High-Rate and Efficient Ethylene Electrosynthesis Using a Catalyst/Promoter/Transport Layer Ozden, Adnan; Li, Fengwang; Garcı́a de Arquer, F. Pelayo ACS Energy Letters, Vol. 5, Issue 9 https://doi.org/10.1021/acsenergylett.0c01266	journal	August 2020
pH Matters When Reducing CO ₂ in an Electrochemical Flow Cell Zhang, Zishuai; Melo, Luke; Jansonius, Ryan P. ACS Energy Letters, Vol. 5, Issue 10 https://doi.org/10.1021/acsenergylett.0c01606	journal	September 2020
Gas-Diffusion Electrodes for Carbon Dioxide Reduction: A New Paradigm Higgins, Drew; Hahn, Christopher; Xiang, Chengxiang ACS Energy Letters, Vol. 4, Issue 1 https://doi.org/10.1021/acsenergylett.8b02035	journal	December 2018
Introductory Guide to Assembling and Operating Gas Diffusion Electrodes for Electrochemical CO ₂ Reduction Liu, Kai; Smith, Wilson A.; Burdyny, Thomas ACS Energy Letters, Vol. 4, Issue 3 https://doi.org/10.1021/acsenergylett.9b00137	journal	February 2019
Along the Channel Gradients Impact on the Spatioactivity of Gas Diffusion Electrodes at High Conversions during CO ₂ Electroreduction Kas, Recep; Star, Andrew G.; Yang, Kailun ACS Sustainable Chemistry & Engineering, Vol. 9, Issue 3 https://doi.org/10.1021/acssuschemeng.0c07694	journal	January 2021
Tin Oxide Dependence of the CO ₂ Reduction Efficiency on Tin Electrodes and Enhanced Activity for Tin/Tin Oxide Thin-Film Catalysts Chen, Yihong; Kanan, Matthew W. Journal of the American Chemical Society, Vol. 134, Issue 4 https://doi.org/10.1021/ja2108799	journal	January 2012
Nanostructured Tin Catalysts for Selective Electrochemical Reduction of Carbon Dioxide to Formate Zhang, Sheng; Kang, Peng; Meyer, Thomas J. Journal of the American Chemical Society, Vol. 136, Issue 5 https://doi.org/10.1021/ja4113885	journal	January 2014
The Central Role of Bicarbonate in the Electrochemical Reduction of Carbon Dioxide on Gold Dunwell, Marco; Lu, Qi; Heyes, Jeffrey M. Journal of the American Chemical Society, Vol. 139, Issue 10 https://doi.org/10.1021/jacs.6b13287	journal	March 2017
Bicarbonate Is Not a General Acid in Au-Catalyzed CO ₂ Electroreduction Wuttig, Anna; Yoon, Youngmin; Ryu, Jaeyune Journal of the American Chemical Society, Vol. 139, Issue 47 https://doi.org/10.1021/jacs.7b08345	journal	November 2017
Direct Observation on Reaction Intermediates and the Role of Bicarbonate Anions in CO ₂ Electrochemical Reduction Reaction on Cu Surfaces Zhu, Shangqian; Jiang, Bei; Cai, Wen-Bin Journal of the American Chemical Society, Vol. 139, Issue 44 https://doi.org/10.1021/jacs.7b10462	journal	October 2017
Formic-acid-induced depolymerization of oxidized lignin to aromatics Rahimi, Alireza; Ulbrich, Arne; Coon, Joshua J. Nature, Vol. 515, Issue 7526, p. 249-252 https://doi.org/10.1038/nature13867	journal	November 2014
Molecular tuning of CO2-to-ethylene conversion Li, Fengwang; Thevenon, Arnaud; Rosas-Hernández, Alonso Nature, Vol. 577, Issue 7791 https://doi.org/10.1038/s41586-019-1782-2	journal	November 2019
The effect of electrolyte composition on the electroreduction of CO ₂ to CO on Ag based gas diffusion electrodes Verma, Sumit; Lu, Xun; Ma, Sichao Physical Chemistry Chemical Physics, Vol. 18, Issue 10 https://doi.org/10.1039/C5CP05665A	journal	January 2016
Modeling gas-diffusion electrodes for CO ₂ reduction Weng, Lien-Chun; Bell, Alexis T.; Weber, Adam Z. Physical Chemistry Chemical Physics, Vol. 20, Issue 25 https://doi.org/10.1039/C8CP01319E	journal	January 2018
CO ₂ reduction on gas-diffusion electrodes and why catalytic performance must be assessed at commercially-relevant conditions Burdyny, Thomas; Smith, Wilson A. Energy & Environmental Science, Vol. 12, Issue 5 https://doi.org/10.1039/C8EE03134G	journal	January 2019
New challenges of electrokinetic studies in investigating the reaction mechanism of electrochemical CO ₂ reduction Lee, Chan Woo; Cho, Nam Heon; Im, Sang Won Journal of Materials Chemistry A, Vol. 6, Issue 29 https://doi.org/10.1039/C8TA03480J	journal	January 2018
Towards membrane-electrode assembly systems for CO ₂ reduction: a modeling study Weng, Lien-Chun; Bell, Alexis T.; Weber, Adam Z. Energy & Environmental Science, Vol. 12, Issue 6 https://doi.org/10.1039/C9EE00909D	journal	January 2019
Formic acid, a biomass-derived source of energy and hydrogen for biomass upgrading Valentini, Federica; Kozell, Vadym; Petrucci, Chiara Energy & Environmental Science, Vol. 12, Issue 9 https://doi.org/10.1039/C9EE01747J	journal	January 2019
Catalyst–electrolyte interface chemistry for electrochemical CO ₂ reduction Sa, Young Jin; Lee, Chan Woo; Lee, Si Young Chemical Society Reviews, Vol. 49, Issue 18 https://doi.org/10.1039/D0CS00030B	journal	January 2020
Electrochemical CO ₂ reduction to methane with remarkably high Faradaic efficiency in the presence of a proton permeable membrane Pan, Hanqing; Barile, Christopher J. Energy & Environmental Science, Vol. 13, Issue 10 https://doi.org/10.1039/D0EE02189J	journal	January 2020
Formation of hydrocarbons in the electrochemical reduction of carbon dioxide at a copper electrode in aqueous solution Hori, Yoshio; Murata, Akira; Takahashi, Ryutaro Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 85, Issue 8 https://doi.org/10.1039/f19898502309	journal	January 1989
Mechanistic insights into electrochemical reduction of CO ₂ over Ag using density functional theory and transport models Singh, Meenesh R.; Goodpaster, Jason D.; Weber, Adam Z. Proceedings of the National Academy of Sciences, Vol. 114, Issue 42 https://doi.org/10.1073/pnas.1713164114	journal	October 2017
Strategies in catalysts and electrolyzer design for electrochemical CO ₂ reduction toward C ₂₊ products Fan, Lei; Xia, Chuan; Yang, Fangqi Science Advances, Vol. 6, Issue 8 https://doi.org/10.1126/sciadv.aay3111	journal	February 2020
Ionic Liquid-Mediated Selective Conversion of CO₂ to CO at Low Overpotentials Rosen, B. A.; Salehi-Khojin, A.; Thorson, M. R. Science, Vol. 334, Issue 6056, p. 643-644 https://doi.org/10.1126/science.1209786	journal	September 2011
What would it take for renewably powered electrosynthesis to displace petrochemical processes? De Luna, Phil; Hahn, Christopher; Higgins, Drew Science, Vol. 364, Issue 6438 https://doi.org/10.1126/science.aav3506	journal	April 2019
Synthesis and Characterization of Perfluorinated Anion Exchange Membranes Park, Andrew Michael; Owczarczyk, Zbyslaw R.; Garner, L. E. ECS Transactions, Vol. 80, Issue 8 https://doi.org/10.1149/08008.0957ecst	journal	August 2017
Elucidating the Role of Ionomer in the Performance of Platinum Group Metal-free Catalyst Layer via in situ Electrochemical Diagnostics Wang, Guanxiong; Osmieri, Luigi; Star, Andrew G. Journal of The Electrochemical Society, Vol. 167, Issue 4 https://doi.org/10.1149/1945-7111/ab7aa1	journal	January 2020
Genome-scale reconstruction and in silico analysis of the Ralstonia eutropha H16 for polyhydroxyalkanoate synthesis, lithoautotrophic growth, and 2-methyl citric acid production Park, Jong; Kim, Tae; Lee, Sang BMC Systems Biology, Vol. 5, Issue 1 https://doi.org/10.1186/1752-0509-5-101	journal	January 2011
Silage review: Recent advances and future uses of silage additives Muck, R. E.; Nadeau, E. M. G.; McAllister, T. A. Journal of Dairy Science, Vol. 101, Issue 5 https://doi.org/10.3168/jds.2017-13839	journal	May 2018
Carbon Dioxide and Water Electrolysis Using New Alkaline Stable Anion Membranes Kaczur, Jerry J.; Yang, Hongzhou; Liu, Zengcai Frontiers in Chemistry, Vol. 6 https://doi.org/10.3389/fchem.2018.00263	journal	July 2018
On the Mechanism of Carbon Dioxide Reduction on Sn-Based Electrodes: Insights into the Role of Oxide Surfaces Damas, Giane B.; Miranda, Caetano R.; Sgarbi, Ricardo Catalysts, Vol. 9, Issue 8 https://doi.org/10.3390/catal9080636	journal	July 2019
Direct Electrochemical Reduction of Bicarbonate to Formate Using Tin Catalyst Bonet Navarro, Andreu; Nogalska, Adrianna; Garcia-Valls, Ricard Electrochem, Vol. 2, Issue 1 https://doi.org/10.3390/electrochem2010006	journal	February 2021

Similar Records

Two‐Membrane Dual Non‐Aqueous/Aqueous Electrolyte Flow Cell Operation for Electrochemical Conversion of CO₂ to Methyl Formate

Journal Article · Sun Nov 05 23:00:00 EST 2023 · ChemSusChem · OSTI ID:2575879

SO₂-Induced Selectivity Change in CO₂ Electroreduction

Journal Article · Mon Jun 03 00:00:00 EDT 2019 · Journal of the American Chemical Society · OSTI ID:1712670

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO2 catalyst selectivity
CO2 reduction
catholyte
electrocatalyst microenvironment
electrons to molecules
ionomer binder materials
modeling

The effect of catholyte and catalyst layer binders on CO2 electroreduction selectivity

Citation Formats

References (51)

Similar Records

Related Subjects

The effect of catholyte and catalyst layer binders on CO₂ electroreduction selectivity