Carbon monoxide electroreduction as an emerging platform for carbon utilization
Abstract
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.
- Authors:
-
[1];
[2];
[1]
- Univ. of Delaware, Newark, DE (United States)
- Lectrolyst, Newark, DE (United States)
- Publication Date:
- Research Org.:
- Univ. of Delaware, Newark, DE (United States)
- Sponsoring Org.:
- USDOE Office of Fossil Energy (FE)
- OSTI Identifier:
- 1712667
- Grant/Contract Number:
- FE0029868
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Catalysis
- Additional Journal Information:
- Journal Volume: 2; Journal Issue: 12; Journal ID: ISSN 2520-1158
- Publisher:
- Springer Nature
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; carbon dioxide; carbon monoxide; electrocatalysts; electrochemical reduction; chemical engineering; energy; heterogeneous catalysis
Citation Formats
Jouny, Matthew, Hutchings, Gregory S., and Jiao, Feng. Carbon monoxide electroreduction as an emerging platform for carbon utilization. United States: N. p., 2019.
Web. doi:10.1038/s41929-019-0388-2.
Jouny, Matthew, Hutchings, Gregory S., & Jiao, Feng. Carbon monoxide electroreduction as an emerging platform for carbon utilization. United States. https://doi.org/10.1038/s41929-019-0388-2
Jouny, Matthew, Hutchings, Gregory S., and Jiao, Feng. Mon .
"Carbon monoxide electroreduction as an emerging platform for carbon utilization". United States. https://doi.org/10.1038/s41929-019-0388-2. https://www.osti.gov/servlets/purl/1712667.
@article{osti_1712667,
title = {Carbon monoxide electroreduction as an emerging platform for carbon utilization},
author = {Jouny, Matthew and Hutchings, Gregory S. and Jiao, Feng},
abstractNote = {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.},
doi = {10.1038/s41929-019-0388-2},
journal = {Nature Catalysis},
number = 12,
volume = 2,
place = {United States},
year = {Mon Dec 09 00:00:00 EST 2019},
month = {Mon Dec 09 00:00:00 EST 2019}
}
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Works referenced in this record:
Net-zero emissions energy systems
journal, June 2018
- Davis, Steven J.; Lewis, Nathan S.; Shaner, Matthew
- Science, Vol. 360, Issue 6396
Terawatt-scale photovoltaics: Trajectories and challenges
journal, April 2017
- Haegel, Nancy M.; Margolis, Robert; Buonassisi, Tonio
- Science, Vol. 356, Issue 6334
Climate change mitigation potential of carbon capture and utilization in the chemical industry
journal, May 2019
- Kätelhön, Arne; Meys, Raoul; Deutz, Sarah
- Proceedings of the National Academy of Sciences, Vol. 116, Issue 23
What would it take for renewably powered electrosynthesis to displace petrochemical processes?
journal, April 2019
- De Luna, Phil; Hahn, Christopher; Higgins, Drew
- Science, Vol. 364, Issue 6438
Progress toward Commercial Application of Electrochemical Carbon Dioxide Reduction
journal, November 2018
- Chen, Chi; Khosrowabadi Kotyk, Juliet F.; Sheehan, Stafford W.
- Chem, Vol. 4, Issue 11
Isolated Ni single atoms in graphene nanosheets for high-performance CO 2 reduction
journal, January 2018
- Jiang, Kun; Siahrostami, Samira; Zheng, Tingting
- Energy & Environmental Science, Vol. 11, Issue 4
High Rate, Selective, and Stable Electroreduction of CO 2 to CO in Basic and Neutral Media
journal, October 2018
- Dinh, Cao-Thang; García de Arquer, F. Pelayo; Sinton, David
- ACS Energy Letters, Vol. 3, Issue 11
CO 2 Electrolysis to CO and O 2 at High Selectivity, Stability and Efficiency Using Sustainion Membranes
journal, January 2018
- Liu, Zengcai; Yang, Hongzhou; Kutz, Robert
- Journal of The Electrochemical Society, Vol. 165, Issue 15
Insights into the Low Overpotential Electroreduction of CO 2 to CO on a Supported Gold Catalyst in an Alkaline Flow Electrolyzer
journal, November 2017
- Verma, Sumit; Hamasaki, Yuki; Kim, Chaerin
- ACS Energy Letters, Vol. 3, Issue 1
CO 2 Electroreduction from Carbonate Electrolyte
journal, May 2019
- Li, Yuguang C.; Lee, Geonhui; Yuan, Tiange
- ACS Energy Letters, Vol. 4, Issue 6
General Techno-Economic Analysis of CO 2 Electrolysis Systems
journal, February 2018
- Jouny, Matthew; Luc, Wesley; Jiao, Feng
- Industrial & Engineering Chemistry Research, Vol. 57, Issue 6
Understanding the Roadmap for Electrochemical Reduction of CO 2 to Multi-Carbon Oxygenates and Hydrocarbons on Copper-Based Catalysts
journal, April 2019
- Zheng, Yao; Vasileff, Anthony; Zhou, Xianlong
- Journal of the American Chemical Society, Vol. 141, Issue 19
Recent Advances in CO 2 Reduction Electrocatalysis on Copper
journal, June 2018
- Raciti, David; Wang, Chao
- ACS Energy Letters, Vol. 3, Issue 7
CO Electroreduction: Current Development and Understanding of Cu-Based Catalysts
journal, November 2018
- Zhang, Haochen; Li, Jing; Cheng, Mu-Jeng
- ACS Catalysis, Vol. 9, Issue 1
High-rate electroreduction of carbon monoxide to multi-carbon products
journal, August 2018
- Jouny, Matthew; Luc, Wesley; Jiao, Feng
- Nature Catalysis, Vol. 1, Issue 10
Two-dimensional copper nanosheets for electrochemical reduction of carbon monoxide to acetate
journal, April 2019
- Luc, Wesley; Fu, Xianbiao; Shi, Jianjian
- Nature Catalysis, Vol. 2, Issue 5
Carbon Monoxide Gas Diffusion Electrolysis that Produces Concentrated C2 Products with High Single-Pass Conversion
journal, January 2019
- Ripatti, Donald S.; Veltman, Thomas R.; Kanan, Matthew W.
- Joule, Vol. 3, Issue 1
Copper nanocavities confine intermediates for efficient electrosynthesis of C3 alcohol fuels from carbon monoxide
journal, October 2018
- Zhuang, Tao-Tao; Pang, Yuanjie; Liang, Zhi-Qin
- Nature Catalysis, Vol. 1, Issue 12
Efficient electrocatalytic conversion of carbon monoxide to propanol using fragmented copper
journal, February 2019
- Pang, Yuanjie; Li, Jun; Wang, Ziyun
- Nature Catalysis, Vol. 2, Issue 3
Formation of carbon–nitrogen bonds in carbon monoxide electrolysis
journal, August 2019
- Jouny, Matthew; Lv, Jing-Jing; Cheng, Tao
- Nature Chemistry, Vol. 11, Issue 9
CO 2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface
journal, May 2018
- Dinh, Cao-Thang; Burdyny, Thomas; Kibria, Md Golam
- Science, Vol. 360, Issue 6390
Nanoporous Copper Films by Additive-Controlled Electrodeposition: CO 2 Reduction Catalysis
journal, April 2017
- Hoang, Thao T. H.; Ma, Sichao; Gold, Jake I.
- ACS Catalysis, Vol. 7, Issue 5
Nanoporous Copper–Silver Alloys by Additive-Controlled Electrodeposition for the Selective Electroreduction of CO 2 to Ethylene and Ethanol
journal, April 2018
- Hoang, Thao T. H.; Verma, Sumit; Ma, Sichao
- Journal of the American Chemical Society, Vol. 140, Issue 17
One-step electrosynthesis of ethylene and ethanol from CO2 in an alkaline electrolyzer
journal, January 2016
- Ma, Sichao; Sadakiyo, Masaaki; Luo, Raymond
- Journal of Power Sources, Vol. 301
A Highly Porous Copper Electrocatalyst for Carbon Dioxide Reduction
journal, October 2018
- Lv, Jing-Jing; Jouny, Matthew; Luc, Wesley
- Advanced Materials, Vol. 30, Issue 49
Towards membrane-electrode assembly systems for CO 2 reduction: a modeling study
journal, January 2019
- Weng, Lien-Chun; Bell, Alexis T.; Weber, Adam Z.
- Energy & Environmental Science, Vol. 12, Issue 6
Electrolysis of CO 2 to Syngas in Bipolar Membrane-Based Electrochemical Cells
journal, November 2016
- Li, Yuguang C.; Zhou, Dekai; Yan, Zhifei
- ACS Energy Letters, Vol. 1, Issue 6
Selective Electroreduction of CO 2 to C2 Products over Cu 3 N‐Derived Cu Nanowires
journal, March 2019
- Mi, Yuying; Shen, Sibo; Peng, Xianyun
- ChemElectroChem, Vol. 6, Issue 9
Catalyst electro-redeposition controls morphology and oxidation state for selective carbon dioxide reduction
journal, January 2018
- De Luna, Phil; Quintero-Bermudez, Rafael; Dinh, Cao-Thang
- Nature Catalysis, Vol. 1, Issue 2
Metal ion cycling of Cu foil for selective C–C coupling in electrochemical CO2 reduction
journal, January 2018
- Jiang, Kun; Sandberg, Robert B.; Akey, Austin J.
- Nature Catalysis, Vol. 1, Issue 2
Selective Electrochemical Reduction of Carbon Dioxide to Ethylene and Ethanol on Copper(I) Oxide Catalysts
journal, March 2015
- Ren, Dan; Deng, Yilin; Handoko, Albertus Denny
- ACS Catalysis, Vol. 5, Issue 5
Plasma-Activated Copper Nanocube Catalysts for Efficient Carbon Dioxide Electroreduction to Hydrocarbons and Alcohols
journal, April 2017
- Gao, Dunfeng; Zegkinoglou, Ioannis; Divins, Nuria J.
- ACS Nano, Vol. 11, Issue 5
Branched Copper Oxide Nanoparticles Induce Highly Selective Ethylene Production by Electrochemical Carbon Dioxide Reduction
journal, April 2019
- Kim, Jinmo; Choi, Woong; Park, Joon Woo
- Journal of the American Chemical Society, Vol. 141, Issue 17
Copper nanoparticle ensembles for selective electroreduction of CO 2 to C 2 –C 3 products
journal, September 2017
- Kim, Dohyung; Kley, Christopher S.; Li, Yifan
- Proceedings of the National Academy of Sciences, Vol. 114, Issue 40
Electrochemical Reduction of CO at a Copper Electrode
journal, September 1997
- Hori, Yoshio; Takahashi, Ryutaro; Yoshinami, Yuzuru
- The Journal of Physical Chemistry B, Vol. 101, Issue 36
Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper
journal, April 2014
- Li, Christina W.; Ciston, Jim; Kanan, Matthew W.
- Nature, Vol. 508, Issue 7497
Probing the Active Surface Sites for CO Reduction on Oxide-Derived Copper Electrocatalysts
journal, July 2015
- Verdaguer-Casadevall, Arnau; Li, Christina W.; Johansson, Tobias P.
- Journal of the American Chemical Society, Vol. 137, Issue 31
Acetaldehyde as an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper
journal, December 2015
- Bertheussen, Erlend; Verdaguer-Casadevall, Arnau; Ravasio, Davide
- Angewandte Chemie International Edition, Vol. 55, Issue 4
Catalysts and Reaction Pathways for the Electrochemical Reduction of Carbon Dioxide
journal, September 2015
- Kortlever, Ruud; Shen, Jing; Schouten, Klaas Jan P.
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 20
Full atomistic reaction mechanism with kinetics for CO reduction on Cu(100) from ab initio molecular dynamics free-energy calculations at 298 K
journal, February 2017
- Cheng, Tao; Xiao, Hai; Goddard, William A.
- Proceedings of the National Academy of Sciences, Vol. 114, Issue 8
Mechanism of CO 2 Reduction at Copper Surfaces: Pathways to C 2 Products
journal, January 2018
- Garza, Alejandro J.; Bell, Alexis T.; Head-Gordon, Martin
- ACS Catalysis, Vol. 8, Issue 2
Electrochemical CO Reduction Builds Solvent Water into Oxygenate Products
journal, July 2018
- Lum, Yanwei; Cheng, Tao; Goddard, William A.
- Journal of the American Chemical Society, Vol. 140, Issue 30
Reaction intermediates during operando electrocatalysis identified from full solvent quantum mechanics molecular dynamics
journal, March 2019
- Cheng, Tao; Fortunelli, Alessandro; Goddard, William A.
- Proceedings of the National Academy of Sciences, Vol. 116, Issue 16
The Importance of Cannizzaro-Type Reactions during Electrocatalytic Reduction of Carbon Dioxide
journal, January 2017
- Birdja, Yuvraj Y.; Koper, Marc T. M.
- Journal of the American Chemical Society, Vol. 139, Issue 5
Electrochemical CO 2 Reduction over Compressively Strained CuAg Surface Alloys with Enhanced Multi-Carbon Oxygenate Selectivity
journal, October 2017
- Clark, Ezra L.; Hahn, Christopher; Jaramillo, Thomas F.
- Journal of the American Chemical Society, Vol. 139, Issue 44
Explaining the Incorporation of Oxygen Derived from Solvent Water into the Oxygenated Products of CO Reduction over Cu
journal, February 2019
- Clark, Ezra L.; Wong, Jonathan; Garza, Alejandro J.
- Journal of the American Chemical Society, Vol. 141, Issue 10
Direct Observation of the Local Reaction Environment during the Electrochemical Reduction of CO 2
journal, April 2018
- Clark, Ezra L.; Bell, Alexis T.
- Journal of the American Chemical Society, Vol. 140, Issue 22
Electrolytic CO 2 Reduction in a Flow Cell
journal, March 2018
- Weekes, David M.; Salvatore, Danielle A.; Reyes, Angelica
- Accounts of Chemical Research, Vol. 51, Issue 4
Gas-Diffusion Electrodes for Carbon Dioxide Reduction: A New Paradigm
journal, December 2018
- Higgins, Drew; Hahn, Christopher; Xiang, Chengxiang
- ACS Energy Letters, Vol. 4, Issue 1
Microfluidic Reactor for the Electrochemical Reduction of Carbon Dioxide: The Effect of pH
journal, January 2010
- Whipple, Devin T.; Finke, Eryn C.; Kenis, Paul J. A.
- Electrochemical and Solid-State Letters, Vol. 13, Issue 9
Boosting the Single-Pass Conversion for Renewable Chemical Electrosynthesis
journal, January 2019
- Dinh, Cao-Thang; Li, Yuguang C.; Sargent, Edward H.
- Joule, Vol. 3, Issue 1
Electrochemical conversion of CO2 to formic acid utilizing Sustainion™ membranes
journal, July 2017
- Yang, Hongzhou; Kaczur, Jerry J.; Sajjad, Syed Dawar
- Journal of CO2 Utilization, Vol. 20
Product Distributions and Efficiencies for Ethanol Oxidation in a Proton Exchange Membrane Electrolysis Cell
journal, January 2017
- Altarawneh, Rakan M.; Pickup, Peter G.
- Journal of The Electrochemical Society, Vol. 164, Issue 7
SO 2 -Induced Selectivity Change in CO 2 Electroreduction
journal, June 2019
- Luc, Wesley; Ko, Byung Hee; Kattel, Shyam
- Journal of the American Chemical Society, Vol. 141, Issue 25
Co-electrolysis of CO2 and glycerol as a pathway to carbon chemicals with improved technoeconomics due to low electricity consumption
journal, April 2019
- Verma, Sumit; Lu, Shawn; Kenis, Paul J. A.
- Nature Energy, Vol. 4, Issue 6
Acetaldehyde as an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper
journal, December 2015
- Bertheussen, Erlend; Verdaguer-Casadevall, Arnau; Ravasio, Davide
- Angewandte Chemie, Vol. 128, Issue 4
Carbon Monoxide Gas Diffusion Electrolysis that Produces Concentrated C2 Products with High Single-Pass Conversion
journal, October 2019
- Ripatti, Donald S.; Veltman, Thomas R.; Kanan, Matthew W.
- Joule, Vol. 3, Issue 10
Acetaldehyde As an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper
journal, April 2016
- Bertheussen, Erlend; Verdaguer-Casdevall, Arnau; Ravasio, Davide
- ECS Meeting Abstracts, Vol. MA2016-01, Issue 38