Modulating Oxygen Affinity to Enhance Liquid Products for the Electrochemical Reduction of Carbon Monoxide
ABSTRACT Electrocatalytic CO reduction (COR) offers a promising alternative approach for synthesizing valuable chemicals, potentially at a lower carbon intensity as compared to conventional chemical production. Cu‐based catalysts have shown encouraging selectivity and activity toward multi‐carbon (C...
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| Format: | Article |
| Language: | English |
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Wiley
2025-04-01
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| Series: | SmartMat |
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| Online Access: | https://doi.org/10.1002/smm2.70010 |
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| author | Jiayi Chen Juan Manuel Arce‐Ramos Ioannis Katsounaros Emiel deSmit Saifudin M. Abubakar Yanwei Lum Jia Zhang Lei Wang |
| author_facet | Jiayi Chen Juan Manuel Arce‐Ramos Ioannis Katsounaros Emiel deSmit Saifudin M. Abubakar Yanwei Lum Jia Zhang Lei Wang |
| author_sort | Jiayi Chen |
| collection | DOAJ |
| description | ABSTRACT Electrocatalytic CO reduction (COR) offers a promising alternative approach for synthesizing valuable chemicals, potentially at a lower carbon intensity as compared to conventional chemical production. Cu‐based catalysts have shown encouraging selectivity and activity toward multi‐carbon (C2+) products, albeit typically in the form of a mixture. Steering COR selectivity toward specific types of C2+ products, such as liquid products with high energy density, remains a challenge. In this study, we developed a Cu/Zn bimetallic catalyst composite and demonstrated enhanced selectivity toward liquid products as compared to reference CuO and Cu‐based catalysts, approaching 60% at a high current density of 300 mA/cm2. Our investigation highlights that the introduction of Zn promoted the emergence of a Cu/Zn heterojunction interface during COR. Density functional theory simulations were used to rationalize the observed differences in selectivity, revealing that interface plays a crucial role in diminishing the oxygen adsorption at the Cu‐sites and modifying the adsorption energy of COR reaction intermediates, consequently leading to enhanced selectivity toward liquid products. |
| format | Article |
| id | doaj-art-dfc25e22016d4e3db2bb56aedc1b5269 |
| institution | OA Journals |
| issn | 2688-819X |
| language | English |
| publishDate | 2025-04-01 |
| publisher | Wiley |
| record_format | Article |
| series | SmartMat |
| spelling | doaj-art-dfc25e22016d4e3db2bb56aedc1b52692025-08-20T02:20:12ZengWileySmartMat2688-819X2025-04-0162n/an/a10.1002/smm2.70010Modulating Oxygen Affinity to Enhance Liquid Products for the Electrochemical Reduction of Carbon MonoxideJiayi Chen0Juan Manuel Arce‐Ramos1Ioannis Katsounaros2Emiel deSmit3Saifudin M. Abubakar4Yanwei Lum5Jia Zhang6Lei Wang7State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry Fuzhou University Fuzhou ChinaInstitute of High Performance Computing (IHPC), Agency for Science, Technology and Research (A*STAR) Singapore SingaporeExxonMobil Chemical Europe LLC Machelen BelgiumExxonMobil Chemical Europe LLC Machelen BelgiumExxonMobil Asia Pacific Pte. Ltd Singapore SingaporeDepartment of Chemical and Biomolecular Engineering National University of Singapore Singapore SingaporeInstitute of High Performance Computing (IHPC), Agency for Science, Technology and Research (A*STAR) Singapore SingaporeDepartment of Chemical and Biomolecular Engineering National University of Singapore Singapore SingaporeABSTRACT Electrocatalytic CO reduction (COR) offers a promising alternative approach for synthesizing valuable chemicals, potentially at a lower carbon intensity as compared to conventional chemical production. Cu‐based catalysts have shown encouraging selectivity and activity toward multi‐carbon (C2+) products, albeit typically in the form of a mixture. Steering COR selectivity toward specific types of C2+ products, such as liquid products with high energy density, remains a challenge. In this study, we developed a Cu/Zn bimetallic catalyst composite and demonstrated enhanced selectivity toward liquid products as compared to reference CuO and Cu‐based catalysts, approaching 60% at a high current density of 300 mA/cm2. Our investigation highlights that the introduction of Zn promoted the emergence of a Cu/Zn heterojunction interface during COR. Density functional theory simulations were used to rationalize the observed differences in selectivity, revealing that interface plays a crucial role in diminishing the oxygen adsorption at the Cu‐sites and modifying the adsorption energy of COR reaction intermediates, consequently leading to enhanced selectivity toward liquid products.https://doi.org/10.1002/smm2.70010C2 liquid productionCO2/CO reductioncopper/zincelectrocatalystsoxygen affinity |
| spellingShingle | Jiayi Chen Juan Manuel Arce‐Ramos Ioannis Katsounaros Emiel deSmit Saifudin M. Abubakar Yanwei Lum Jia Zhang Lei Wang Modulating Oxygen Affinity to Enhance Liquid Products for the Electrochemical Reduction of Carbon Monoxide SmartMat C2 liquid production CO2/CO reduction copper/zinc electrocatalysts oxygen affinity |
| title | Modulating Oxygen Affinity to Enhance Liquid Products for the Electrochemical Reduction of Carbon Monoxide |
| title_full | Modulating Oxygen Affinity to Enhance Liquid Products for the Electrochemical Reduction of Carbon Monoxide |
| title_fullStr | Modulating Oxygen Affinity to Enhance Liquid Products for the Electrochemical Reduction of Carbon Monoxide |
| title_full_unstemmed | Modulating Oxygen Affinity to Enhance Liquid Products for the Electrochemical Reduction of Carbon Monoxide |
| title_short | Modulating Oxygen Affinity to Enhance Liquid Products for the Electrochemical Reduction of Carbon Monoxide |
| title_sort | modulating oxygen affinity to enhance liquid products for the electrochemical reduction of carbon monoxide |
| topic | C2 liquid production CO2/CO reduction copper/zinc electrocatalysts oxygen affinity |
| url | https://doi.org/10.1002/smm2.70010 |
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