Carbon monoxide electroreduction as an emerging platform for carbon utilization

Jouny, Matthew; Hutchings, Gregory S.; Jiao, Feng

doi:10.1038/s41929-019-0388-2

Title: Carbon monoxide electroreduction as an emerging platform for carbon utilization

Journal Article · 08 December 2019 · Nature Catalysis

DOI: https://doi.org/10.1038/s41929-019-0388-2 · OSTI ID:1712667

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Univ. of Delaware, Newark, DE (United States); University of Delaware
Lectrolyst, Newark, DE (United States)
Univ. of Delaware, Newark, DE (United States)

The electrochemical conversion of carbon dioxide to value-added chemical products has been heavily explored as a promising strategy for carbon utilization. However, the direct synthesis of multi-carbon (C₂₊) products suffers from undesired side reactions and relatively low selectivity. Electrochemically converting CO₂ to single-carbon products is much more effective and being commercially deployed. Recent studies have shown that CO can be electrochemically transformed further to C₂₊ at high reaction rates, high C₂₊ selectivity and inherently improved electrolyte stability, raising the prospect of a two-step pathway to transform CO₂. In this Perspective, the progress towards high-rate CO conversion is shown alongside mechanistic insights and device designs that can improve performance even further. Here, a techno-economic analysis of the two-step conversion process and cradle-to-gate lifecycle assessment shows the economic feasibility and improved environmental impact of a high-volume commercial process generating acetic acid and ethylene compared to the current state of the art.

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Research Organization:: Univ. of Delaware, Newark, DE (United States)

Sponsoring Organization:: USDOE Office of Fossil Energy (FE)

Grant/Contract Number:: FE0029868

OSTI ID:: 1712667

Journal Information:: Nature Catalysis, Journal Name: Nature Catalysis Journal Issue: 12 Vol. 2; ISSN 2520-1158

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

References (58)

A Highly Porous Copper Electrocatalyst for Carbon Dioxide Reduction Lv, Jing-Jing; Jouny, Matthew; Luc, Wesley Advanced Materials, Vol. 30, Issue 49 https://doi.org/10.1002/adma.201803111	journal	October 2018
Acetaldehyde as an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper Bertheussen, Erlend; Verdaguer-Casadevall, Arnau; Ravasio, Davide Angewandte Chemie, Vol. 128, Issue 4 https://doi.org/10.1002/ange.201508851	journal	December 2015
Acetaldehyde as an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper Bertheussen, Erlend; Verdaguer-Casadevall, Arnau; Ravasio, Davide Angewandte Chemie International Edition, Vol. 55, Issue 4 https://doi.org/10.1002/anie.201508851	journal	December 2015
Selective Electroreduction of CO ₂ to C2 Products over Cu ₃ N‐Derived Cu Nanowires Mi, Yuying; Shen, Sibo; Peng, Xianyun ChemElectroChem, Vol. 6, Issue 9 https://doi.org/10.1002/celc.201801826	journal	March 2019
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 conversion of CO2 to formic acid utilizing Sustainion™ membranes Yang, Hongzhou; Kaczur, Jerry J.; Sajjad, Syed Dawar Journal of CO2 Utilization, Vol. 20 https://doi.org/10.1016/j.jcou.2017.04.011	journal	July 2017
Carbon Monoxide Gas Diffusion Electrolysis that Produces Concentrated C2 Products with High Single-Pass Conversion Ripatti, Donald S.; Veltman, Thomas R.; Kanan, Matthew W. Joule, Vol. 3, Issue 1 https://doi.org/10.1016/j.joule.2018.10.007	journal	January 2019
Boosting the Single-Pass Conversion for Renewable Chemical Electrosynthesis Dinh, Cao-Thang; Li, Yuguang C.; Sargent, Edward H. Joule, Vol. 3, Issue 1 https://doi.org/10.1016/j.joule.2018.10.021	journal	January 2019
Carbon Monoxide Gas Diffusion Electrolysis that Produces Concentrated C2 Products with High Single-Pass Conversion Ripatti, Donald S.; Veltman, Thomas R.; Kanan, Matthew W. Joule, Vol. 3, Issue 10 https://doi.org/10.1016/j.joule.2019.09.012	journal	October 2019
One-step electrosynthesis of ethylene and ethanol from CO2 in an alkaline electrolyzer Ma, Sichao; Sadakiyo, Masaaki; Luo, Raymond Journal of Power Sources, Vol. 301 https://doi.org/10.1016/j.jpowsour.2015.09.124	journal	January 2016
Electrolytic CO ₂ Reduction in a Flow Cell Weekes, David M.; Salvatore, Danielle A.; Reyes, Angelica Accounts of Chemical Research, Vol. 51, Issue 4 https://doi.org/10.1021/acs.accounts.8b00010	journal	March 2018
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
Catalysts and Reaction Pathways for the Electrochemical Reduction of Carbon Dioxide Kortlever, Ruud; Shen, Jing; Schouten, Klaas Jan P. The Journal of Physical Chemistry Letters, Vol. 6, Issue 20 https://doi.org/10.1021/acs.jpclett.5b01559	journal	September 2015
Nanoporous Copper Films by Additive-Controlled Electrodeposition: CO ₂ Reduction Catalysis Hoang, Thao T. H.; Ma, Sichao; Gold, Jake I. ACS Catalysis, Vol. 7, Issue 5 https://doi.org/10.1021/acscatal.6b03613	journal	April 2017
Mechanism of CO ₂ Reduction at Copper Surfaces: Pathways to C ₂ Products Garza, Alejandro J.; Bell, Alexis T.; Head-Gordon, Martin ACS Catalysis, Vol. 8, Issue 2 https://doi.org/10.1021/acscatal.7b03477	journal	January 2018
CO Electroreduction: Current Development and Understanding of Cu-Based Catalysts Zhang, Haochen; Li, Jing; Cheng, Mu-Jeng ACS Catalysis, Vol. 9, Issue 1 https://doi.org/10.1021/acscatal.8b03780	journal	November 2018
Electrolysis of CO ₂ to Syngas in Bipolar Membrane-Based Electrochemical Cells Li, Yuguang C.; Zhou, Dekai; Yan, Zhifei ACS Energy Letters, Vol. 1, Issue 6 https://doi.org/10.1021/acsenergylett.6b00475	journal	November 2016
Insights into the Low Overpotential Electroreduction of CO ₂ to CO on a Supported Gold Catalyst in an Alkaline Flow Electrolyzer Verma, Sumit; Hamasaki, Yuki; Kim, Chaerin ACS Energy Letters, Vol. 3, Issue 1 https://doi.org/10.1021/acsenergylett.7b01096	journal	November 2017
Recent Advances in CO ₂ Reduction Electrocatalysis on Copper Raciti, David; Wang, Chao ACS Energy Letters, Vol. 3, Issue 7 https://doi.org/10.1021/acsenergylett.8b00553	journal	June 2018
High Rate, Selective, and Stable Electroreduction of CO ₂ to CO in Basic and Neutral Media Dinh, Cao-Thang; García de Arquer, F. Pelayo; Sinton, David ACS Energy Letters, Vol. 3, Issue 11 https://doi.org/10.1021/acsenergylett.8b01734	journal	October 2018
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
CO ₂ Electroreduction from Carbonate Electrolyte Li, Yuguang C.; Lee, Geonhui; Yuan, Tiange ACS Energy Letters, Vol. 4, Issue 6 https://doi.org/10.1021/acsenergylett.9b00975	journal	May 2019
Plasma-Activated Copper Nanocube Catalysts for Efficient Carbon Dioxide Electroreduction to Hydrocarbons and Alcohols Gao, Dunfeng; Zegkinoglou, Ioannis; Divins, Nuria J. ACS Nano, Vol. 11, Issue 5 https://doi.org/10.1021/acsnano.7b01257	journal	April 2017
Selective Electrochemical Reduction of Carbon Dioxide to Ethylene and Ethanol on Copper(I) Oxide Catalysts Ren, Dan; Deng, Yilin; Handoko, Albertus Denny ACS Catalysis, Vol. 5, Issue 5 https://doi.org/10.1021/cs502128q	journal	March 2015
Probing the Active Surface Sites for CO Reduction on Oxide-Derived Copper Electrocatalysts Verdaguer-Casadevall, Arnau; Li, Christina W.; Johansson, Tobias P. Journal of the American Chemical Society, Vol. 137, Issue 31 https://doi.org/10.1021/jacs.5b06227	journal	July 2015
The Importance of Cannizzaro-Type Reactions during Electrocatalytic Reduction of Carbon Dioxide Birdja, Yuvraj Y.; Koper, Marc T. M. Journal of the American Chemical Society, Vol. 139, Issue 5 https://doi.org/10.1021/jacs.6b12008	journal	January 2017
Electrochemical CO ₂ Reduction over Compressively Strained CuAg Surface Alloys with Enhanced Multi-Carbon Oxygenate Selectivity Clark, Ezra L.; Hahn, Christopher; Jaramillo, Thomas F. Journal of the American Chemical Society, Vol. 139, Issue 44 https://doi.org/10.1021/jacs.7b08607	journal	October 2017
Nanoporous Copper–Silver Alloys by Additive-Controlled Electrodeposition for the Selective Electroreduction of CO ₂ to Ethylene and Ethanol Hoang, Thao T. H.; Verma, Sumit; Ma, Sichao Journal of the American Chemical Society, Vol. 140, Issue 17 https://doi.org/10.1021/jacs.8b01868	journal	April 2018
Electrochemical CO Reduction Builds Solvent Water into Oxygenate Products Lum, Yanwei; Cheng, Tao; Goddard, William A. Journal of the American Chemical Society, Vol. 140, Issue 30 https://doi.org/10.1021/jacs.8b03986	journal	July 2018
Direct Observation of the Local Reaction Environment during the Electrochemical Reduction of CO ₂ Clark, Ezra L.; Bell, Alexis T. Journal of the American Chemical Society, Vol. 140, Issue 22 https://doi.org/10.1021/jacs.8b04058	journal	April 2018
Explaining the Incorporation of Oxygen Derived from Solvent Water into the Oxygenated Products of CO Reduction over Cu Clark, Ezra L.; Wong, Jonathan; Garza, Alejandro J. Journal of the American Chemical Society, Vol. 141, Issue 10 https://doi.org/10.1021/jacs.8b13201	journal	February 2019
Branched Copper Oxide Nanoparticles Induce Highly Selective Ethylene Production by Electrochemical Carbon Dioxide Reduction Kim, Jinmo; Choi, Woong; Park, Joon Woo Journal of the American Chemical Society, Vol. 141, Issue 17 https://doi.org/10.1021/jacs.9b00911	journal	April 2019
Understanding the Roadmap for Electrochemical Reduction of CO ₂ to Multi-Carbon Oxygenates and Hydrocarbons on Copper-Based Catalysts Zheng, Yao; Vasileff, Anthony; Zhou, Xianlong Journal of the American Chemical Society, Vol. 141, Issue 19 https://doi.org/10.1021/jacs.9b02124	journal	April 2019
SO ₂ -Induced Selectivity Change in CO ₂ Electroreduction Luc, Wesley; Ko, Byung Hee; Kattel, Shyam Journal of the American Chemical Society, Vol. 141, Issue 25 https://doi.org/10.1021/jacs.9b03215	journal	June 2019
Electrochemical Reduction of CO at a Copper Electrode Hori, Yoshio; Takahashi, Ryutaro; Yoshinami, Yuzuru The Journal of Physical Chemistry B, Vol. 101, Issue 36 https://doi.org/10.1021/jp970284i	journal	September 1997
Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper Li, Christina W.; Ciston, Jim; Kanan, Matthew W. Nature, Vol. 508, Issue 7497 https://doi.org/10.1038/nature13249	journal	April 2014
Formation of carbon–nitrogen bonds in carbon monoxide electrolysis Jouny, Matthew; Lv, Jing-Jing; Cheng, Tao Nature Chemistry, Vol. 11, Issue 9 https://doi.org/10.1038/s41557-019-0312-z	journal	August 2019
Co-electrolysis of CO2 and glycerol as a pathway to carbon chemicals with improved technoeconomics due to low electricity consumption Verma, Sumit; Lu, Shawn; Kenis, Paul J. A. Nature Energy, Vol. 4, Issue 6 https://doi.org/10.1038/s41560-019-0374-6	journal	April 2019
Metal ion cycling of Cu foil for selective C–C coupling in electrochemical CO2 reduction Jiang, Kun; Sandberg, Robert B.; Akey, Austin J. Nature Catalysis, Vol. 1, Issue 2 https://doi.org/10.1038/s41929-017-0009-x	journal	January 2018
Catalyst electro-redeposition controls morphology and oxidation state for selective carbon dioxide reduction De Luna, Phil; Quintero-Bermudez, Rafael; Dinh, Cao-Thang Nature Catalysis, Vol. 1, Issue 2 https://doi.org/10.1038/s41929-017-0018-9	journal	January 2018
High-rate electroreduction of carbon monoxide to multi-carbon products Jouny, Matthew; Luc, Wesley; Jiao, Feng Nature Catalysis, Vol. 1, Issue 10 https://doi.org/10.1038/s41929-018-0133-2	journal	August 2018
Copper nanocavities confine intermediates for efficient electrosynthesis of C3 alcohol fuels from carbon monoxide Zhuang, Tao-Tao; Pang, Yuanjie; Liang, Zhi-Qin Nature Catalysis, Vol. 1, Issue 12 https://doi.org/10.1038/s41929-018-0168-4	journal	October 2018
Efficient electrocatalytic conversion of carbon monoxide to propanol using fragmented copper Pang, Yuanjie; Li, Jun; Wang, Ziyun Nature Catalysis, Vol. 2, Issue 3 https://doi.org/10.1038/s41929-019-0225-7	journal	February 2019
Two-dimensional copper nanosheets for electrochemical reduction of carbon monoxide to acetate Luc, Wesley; Fu, Xianbiao; Shi, Jianjian Nature Catalysis, Vol. 2, Issue 5 https://doi.org/10.1038/s41929-019-0269-8	journal	April 2019
Isolated Ni single atoms in graphene nanosheets for high-performance CO ₂ reduction Jiang, Kun; Siahrostami, Samira; Zheng, Tingting Energy & Environmental Science, Vol. 11, Issue 4 https://doi.org/10.1039/C7EE03245E	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
Full atomistic reaction mechanism with kinetics for CO reduction on Cu(100) from ab initio molecular dynamics free-energy calculations at 298 K Cheng, Tao; Xiao, Hai; Goddard, William A. Proceedings of the National Academy of Sciences, Vol. 114, Issue 8 https://doi.org/10.1073/pnas.1612106114	journal	February 2017
Copper nanoparticle ensembles for selective electroreduction of CO ₂ to C ₂ –C ₃ products Kim, Dohyung; Kley, Christopher S.; Li, Yifan Proceedings of the National Academy of Sciences, Vol. 114, Issue 40 https://doi.org/10.1073/pnas.1711493114	journal	September 2017
Climate change mitigation potential of carbon capture and utilization in the chemical industry Kätelhön, Arne; Meys, Raoul; Deutz, Sarah Proceedings of the National Academy of Sciences, Vol. 116, Issue 23 https://doi.org/10.1073/pnas.1821029116	journal	May 2019
Reaction intermediates during operando electrocatalysis identified from full solvent quantum mechanics molecular dynamics Cheng, Tao; Fortunelli, Alessandro; Goddard, William A. Proceedings of the National Academy of Sciences, Vol. 116, Issue 16 https://doi.org/10.1073/pnas.1821709116	journal	March 2019
Terawatt-scale photovoltaics: Trajectories and challenges Haegel, Nancy M.; Margolis, Robert; Buonassisi, Tonio Science, Vol. 356, Issue 6334 https://doi.org/10.1126/science.aal1288	journal	April 2017
CO ₂ electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface Dinh, Cao-Thang; Burdyny, Thomas; Kibria, Md Golam Science, Vol. 360, Issue 6390 https://doi.org/10.1126/science.aas9100	journal	May 2018
Net-zero emissions energy systems Davis, Steven J.; Lewis, Nathan S.; Shaner, Matthew Science, Vol. 360, Issue 6396 https://doi.org/10.1126/science.aas9793	journal	June 2018
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
Microfluidic Reactor for the Electrochemical Reduction of Carbon Dioxide: The Effect of pH Whipple, Devin T.; Finke, Eryn C.; Kenis, Paul J. A. Electrochemical and Solid-State Letters, Vol. 13, Issue 9 https://doi.org/10.1149/1.3456590	journal	January 2010
Product Distributions and Efficiencies for Ethanol Oxidation in a Proton Exchange Membrane Electrolysis Cell Altarawneh, Rakan M.; Pickup, Peter G. Journal of The Electrochemical Society, Vol. 164, Issue 7 https://doi.org/10.1149/2.0051709jes	journal	January 2017
CO ₂ Electrolysis to CO and O ₂ at High Selectivity, Stability and Efficiency Using Sustainion Membranes Liu, Zengcai; Yang, Hongzhou; Kutz, Robert Journal of The Electrochemical Society, Vol. 165, Issue 15 https://doi.org/10.1149/2.0501815jes	journal	January 2018
Acetaldehyde As an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper Bertheussen, Erlend; Verdaguer-Casdevall, Arnau; Ravasio, Davide ECS Meeting Abstracts, Vol. MA2016-01, Issue 38 https://doi.org/10.1149/ma2016-01/38/1940	journal	April 2016

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
carbon dioxide
carbon monoxide
chemical engineering
electrocatalysts
electrochemical reduction
energy
heterogeneous catalysis

Title: Carbon monoxide electroreduction as an emerging platform for carbon utilization

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