Cargando…
CO(2) electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment
Electrochemical CO(2) reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate CO(2) electroreduction in strongly acidic electrolyte (pH ≤ 1) on electrochemically reduced porous Cu nanosheets by combining the conf...
Autores principales: | , , , , , , , , , , |
---|---|
Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2022
|
Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9734127/ https://www.ncbi.nlm.nih.gov/pubmed/36494381 http://dx.doi.org/10.1038/s41467-022-35415-x |
_version_ | 1784846521027526656 |
---|---|
author | Ma, Zesong Yang, Zhilong Lai, Wenchuan Wang, Qiyou Qiao, Yan Tao, Haolan Lian, Cheng Liu, Min Ma, Chao Pan, Anlian Huang, Hongwen |
author_facet | Ma, Zesong Yang, Zhilong Lai, Wenchuan Wang, Qiyou Qiao, Yan Tao, Haolan Lian, Cheng Liu, Min Ma, Chao Pan, Anlian Huang, Hongwen |
author_sort | Ma, Zesong |
collection | PubMed |
description | Electrochemical CO(2) reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate CO(2) electroreduction in strongly acidic electrolyte (pH ≤ 1) on electrochemically reduced porous Cu nanosheets by combining the confinement effect and cation effect to synergistically modulate the local microenvironment. A Faradaic efficiency of 83.7 ± 1.4% and partial current density of 0.56 ± 0.02 A cm(−2), single-pass carbon efficiency of 54.4%, and stable electrolysis of 30 h in a flow cell are demonstrated for multicarbon products in a strongly acidic aqueous electrolyte consisting of sulfuric acid and KCl with pH ≤ 1. Mechanistically, the accumulated species (e.g., K(+) and OH(−)) on the Helmholtz plane account for the selectivity and activity toward multicarbon products by kinetically reducing the proton coverage and thermodynamically favoring the CO(2) conversion. We find that the K(+) cations facilitate C-C coupling through local interaction between K(+) and the key intermediate *OCCO. |
format | Online Article Text |
id | pubmed-9734127 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-97341272022-12-11 CO(2) electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment Ma, Zesong Yang, Zhilong Lai, Wenchuan Wang, Qiyou Qiao, Yan Tao, Haolan Lian, Cheng Liu, Min Ma, Chao Pan, Anlian Huang, Hongwen Nat Commun Article Electrochemical CO(2) reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate CO(2) electroreduction in strongly acidic electrolyte (pH ≤ 1) on electrochemically reduced porous Cu nanosheets by combining the confinement effect and cation effect to synergistically modulate the local microenvironment. A Faradaic efficiency of 83.7 ± 1.4% and partial current density of 0.56 ± 0.02 A cm(−2), single-pass carbon efficiency of 54.4%, and stable electrolysis of 30 h in a flow cell are demonstrated for multicarbon products in a strongly acidic aqueous electrolyte consisting of sulfuric acid and KCl with pH ≤ 1. Mechanistically, the accumulated species (e.g., K(+) and OH(−)) on the Helmholtz plane account for the selectivity and activity toward multicarbon products by kinetically reducing the proton coverage and thermodynamically favoring the CO(2) conversion. We find that the K(+) cations facilitate C-C coupling through local interaction between K(+) and the key intermediate *OCCO. Nature Publishing Group UK 2022-12-09 /pmc/articles/PMC9734127/ /pubmed/36494381 http://dx.doi.org/10.1038/s41467-022-35415-x Text en © The Author(s) 2022 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) . |
spellingShingle | Article Ma, Zesong Yang, Zhilong Lai, Wenchuan Wang, Qiyou Qiao, Yan Tao, Haolan Lian, Cheng Liu, Min Ma, Chao Pan, Anlian Huang, Hongwen CO(2) electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment |
title | CO(2) electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment |
title_full | CO(2) electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment |
title_fullStr | CO(2) electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment |
title_full_unstemmed | CO(2) electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment |
title_short | CO(2) electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment |
title_sort | co(2) electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9734127/ https://www.ncbi.nlm.nih.gov/pubmed/36494381 http://dx.doi.org/10.1038/s41467-022-35415-x |
work_keys_str_mv | AT mazesong co2electroreductiontomulticarbonproductsinstronglyacidicelectrolyteviasynergisticallymodulatingthelocalmicroenvironment AT yangzhilong co2electroreductiontomulticarbonproductsinstronglyacidicelectrolyteviasynergisticallymodulatingthelocalmicroenvironment AT laiwenchuan co2electroreductiontomulticarbonproductsinstronglyacidicelectrolyteviasynergisticallymodulatingthelocalmicroenvironment AT wangqiyou co2electroreductiontomulticarbonproductsinstronglyacidicelectrolyteviasynergisticallymodulatingthelocalmicroenvironment AT qiaoyan co2electroreductiontomulticarbonproductsinstronglyacidicelectrolyteviasynergisticallymodulatingthelocalmicroenvironment AT taohaolan co2electroreductiontomulticarbonproductsinstronglyacidicelectrolyteviasynergisticallymodulatingthelocalmicroenvironment AT liancheng co2electroreductiontomulticarbonproductsinstronglyacidicelectrolyteviasynergisticallymodulatingthelocalmicroenvironment AT liumin co2electroreductiontomulticarbonproductsinstronglyacidicelectrolyteviasynergisticallymodulatingthelocalmicroenvironment AT machao co2electroreductiontomulticarbonproductsinstronglyacidicelectrolyteviasynergisticallymodulatingthelocalmicroenvironment AT pananlian co2electroreductiontomulticarbonproductsinstronglyacidicelectrolyteviasynergisticallymodulatingthelocalmicroenvironment AT huanghongwen co2electroreductiontomulticarbonproductsinstronglyacidicelectrolyteviasynergisticallymodulatingthelocalmicroenvironment |