Potential and electric double-layer effect in electrocatalytic urea synthesis
Electrochemical synthesis is a promising way for sustainable urea production, yet the exact mechanism has not been fully revealed. Herein, we explore the mechanism of electrochemical coupling of nitrite and carbon dioxide on Cu surfaces towards urea synthesis on the basis of a constant-potential met...
| Main Authors: | , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2024
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| Online Access: | https://hdl.handle.net/10356/174703 |
| _version_ | 1826125463224844288 |
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| author | Wu, Qian Dai, Chencheng Meng, Fanxu Jiao, Yan Xu, Jason Zhichuan |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Wu, Qian Dai, Chencheng Meng, Fanxu Jiao, Yan Xu, Jason Zhichuan |
| author_sort | Wu, Qian |
| collection | NTU |
| description | Electrochemical synthesis is a promising way for sustainable urea production, yet the exact mechanism has not been fully revealed. Herein, we explore the mechanism of electrochemical coupling of nitrite and carbon dioxide on Cu surfaces towards urea synthesis on the basis of a constant-potential method combined with an implicit solvent model. The working electrode potential, which has normally overlooked, is found influential on both the reaction mechanism and activity. The further computational study on the reaction pathways reveals that *CO-NH and *NH-CO-NH as the key intermediates. In addition, through the analysis of turnover frequencies under various potentials, pressures, and temperatures within a microkinetic model, we demonstrate that the activity increases with temperature, and the Cu(100) shows the highest efficiency towards urea synthesis among all three Cu surfaces. The electric double-layer capacitance also plays a key role in urea synthesis. Based on these findings, we propose two essential strategies to promote the efficiency of urea synthesis on Cu electrodes: increasing Cu(100) surface ratio and elevating the reaction temperature. |
| first_indexed | 2024-10-01T06:37:01Z |
| format | Journal Article |
| id | ntu-10356/174703 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T06:37:01Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1747032024-04-12T15:48:04Z Potential and electric double-layer effect in electrocatalytic urea synthesis Wu, Qian Dai, Chencheng Meng, Fanxu Jiao, Yan Xu, Jason Zhichuan School of Materials Science and Engineering Interdisciplinary Graduate School (IGS) The Cambridge Centre for Advanced Research and Education in Singapore Energy Research Institute @ NTU (ERI@N) Center for Advanced Catalysis Science and Technology Engineering Electrocatalysis Reaction analysis Electrochemical synthesis is a promising way for sustainable urea production, yet the exact mechanism has not been fully revealed. Herein, we explore the mechanism of electrochemical coupling of nitrite and carbon dioxide on Cu surfaces towards urea synthesis on the basis of a constant-potential method combined with an implicit solvent model. The working electrode potential, which has normally overlooked, is found influential on both the reaction mechanism and activity. The further computational study on the reaction pathways reveals that *CO-NH and *NH-CO-NH as the key intermediates. In addition, through the analysis of turnover frequencies under various potentials, pressures, and temperatures within a microkinetic model, we demonstrate that the activity increases with temperature, and the Cu(100) shows the highest efficiency towards urea synthesis among all three Cu surfaces. The electric double-layer capacitance also plays a key role in urea synthesis. Based on these findings, we propose two essential strategies to promote the efficiency of urea synthesis on Cu electrodes: increasing Cu(100) surface ratio and elevating the reaction temperature. Agency for Science, Technology and Research (A*STAR) Ministry of Education (MOE) Published version This work is supported by Singapore Ministry of Education Tier 1 Grant (RG78/22) and A*STAR (Agency for Science, Technology and Research) under its LCERFI program (Award No. U2102d2002). 2024-04-08T02:52:07Z 2024-04-08T02:52:07Z 2024 Journal Article Wu, Q., Dai, C., Meng, F., Jiao, Y. & Xu, J. Z. (2024). Potential and electric double-layer effect in electrocatalytic urea synthesis. Nature Communications, 15(1), 1095-. https://dx.doi.org/10.1038/s41467-024-45522-6 2041-1723 https://hdl.handle.net/10356/174703 10.1038/s41467-024-45522-6 38321031 2-s2.0-85187112171 1 15 1095 en RG78/22 U2102d2002 Nature Communications © The Author(s) 2024. 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/. application/pdf |
| spellingShingle | Engineering Electrocatalysis Reaction analysis Wu, Qian Dai, Chencheng Meng, Fanxu Jiao, Yan Xu, Jason Zhichuan Potential and electric double-layer effect in electrocatalytic urea synthesis |
| title | Potential and electric double-layer effect in electrocatalytic urea synthesis |
| title_full | Potential and electric double-layer effect in electrocatalytic urea synthesis |
| title_fullStr | Potential and electric double-layer effect in electrocatalytic urea synthesis |
| title_full_unstemmed | Potential and electric double-layer effect in electrocatalytic urea synthesis |
| title_short | Potential and electric double-layer effect in electrocatalytic urea synthesis |
| title_sort | potential and electric double layer effect in electrocatalytic urea synthesis |
| topic | Engineering Electrocatalysis Reaction analysis |
| url | https://hdl.handle.net/10356/174703 |
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