Selective electrocatalytic synthesis of urea with nitrate and carbon dioxide
Synthetic nitrogen fertilizer such as urea has been key to increasing crop productivity and feeding a growing population. However, the conventional urea production relies on energy-intensive processes, consuming approximately 2% of annual global energy. Here, we report on a more-sustainable electroc...
| Main Authors: | , , , , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2022
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| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/154705 |
| _version_ | 1826118977780187136 |
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| author | Lv, Chade Zhong, Lixiang Liu, Hengjie Fang, Zhiwei Yan, Chunshuang Chen, Mengxin Kong, Yi Lee, Carmen Liu, Daobin Li, Shuzhou Liu, Jiawei Song, Li Chen, Gang Yan, Qingyu Yu, Guihua |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Lv, Chade Zhong, Lixiang Liu, Hengjie Fang, Zhiwei Yan, Chunshuang Chen, Mengxin Kong, Yi Lee, Carmen Liu, Daobin Li, Shuzhou Liu, Jiawei Song, Li Chen, Gang Yan, Qingyu Yu, Guihua |
| author_sort | Lv, Chade |
| collection | NTU |
| description | Synthetic nitrogen fertilizer such as urea has been key to increasing crop productivity and feeding a growing population. However, the conventional urea production relies on energy-intensive processes, consuming approximately 2% of annual global energy. Here, we report on a more-sustainable electrocatalytic approach that allows for direct and selective synthesis of urea from nitrate and carbon dioxide with an indium hydroxide catalyst at ambient conditions. Remarkably, Faradaic efficiency, nitrogen selectivity and carbon selectivity reach 53.4%, 82.9% and ~100%, respectively. The engineered surface semiconducting behaviour of the catalyst is found to suppress hydrogen evolution reaction. The key step of C–N coupling initiates through the reaction between *NO2 and *CO2 intermediates owing to the low energy barrier on {100} facets. This work suggests an appealing route of urea production and provides deep insight into the underlying chemistry of C–N coupling reaction that could guide sustainable synthesis of other indispensable chemicals. |
| first_indexed | 2024-10-01T04:52:25Z |
| format | Journal Article |
| id | ntu-10356/154705 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T04:52:25Z |
| publishDate | 2022 |
| record_format | dspace |
| spelling | ntu-10356/1547052023-07-14T16:03:27Z Selective electrocatalytic synthesis of urea with nitrate and carbon dioxide Lv, Chade Zhong, Lixiang Liu, Hengjie Fang, Zhiwei Yan, Chunshuang Chen, Mengxin Kong, Yi Lee, Carmen Liu, Daobin Li, Shuzhou Liu, Jiawei Song, Li Chen, Gang Yan, Qingyu Yu, Guihua School of Materials Science and Engineering Engineering::Materials::Energy materials Carbon Dioxide Catalysts Synthetic nitrogen fertilizer such as urea has been key to increasing crop productivity and feeding a growing population. However, the conventional urea production relies on energy-intensive processes, consuming approximately 2% of annual global energy. Here, we report on a more-sustainable electrocatalytic approach that allows for direct and selective synthesis of urea from nitrate and carbon dioxide with an indium hydroxide catalyst at ambient conditions. Remarkably, Faradaic efficiency, nitrogen selectivity and carbon selectivity reach 53.4%, 82.9% and ~100%, respectively. The engineered surface semiconducting behaviour of the catalyst is found to suppress hydrogen evolution reaction. The key step of C–N coupling initiates through the reaction between *NO2 and *CO2 intermediates owing to the low energy barrier on {100} facets. This work suggests an appealing route of urea production and provides deep insight into the underlying chemistry of C–N coupling reaction that could guide sustainable synthesis of other indispensable chemicals. Agency for Science, Technology and Research (A*STAR) Ministry of Education (MOE) National Supercomputing Centre (NSCC) Singapore Accepted version Q.Y. acknowledges funding support from Singapore MOE AcRF Tier 1 grant no. 2020-T1-001-031, Tier 2 grant no. 2017-T2-2-069 and Singapore A*STAR project A19D9a0096. G.Y. acknowledges funding support from the US Department of Energy (grant number: DE-SC0019019) and Welch Foundation Award F-1861. S.L. acknowledges financial support from the Academic Research Fund Tier 1 (RG8/20), Tier 1 (RG104/18) and computing resources from the National Supercomputing Centre Singapore. This work is also supported by the Users with Excellence programme of Hefei Science Center of CAS(2020HSC-UE003). We greatly thank the Facility for Analysis, Characterization, Testing and Simulation (FACTS) of Nanyang Technological University, Singapore, for using their TEM, SEM and XRD equipment. We acknowledge NTU Center of High Field NMR Spectroscopy and Imaging. We also thank the National Synchrotron Radiation Laboratory for help in characterizations. 2022-01-05T06:33:01Z 2022-01-05T06:33:01Z 2021 Journal Article Lv, C., Zhong, L., Liu, H., Fang, Z., Yan, C., Chen, M., Kong, Y., Lee, C., Liu, D., Li, S., Liu, J., Song, L., Chen, G., Yan, Q. & Yu, G. (2021). Selective electrocatalytic synthesis of urea with nitrate and carbon dioxide. Nature Sustainability, 4, 868-876. https://dx.doi.org/10.1038/s41893-021-00741-3 2398-9629 https://hdl.handle.net/10356/154705 10.1038/s41893-021-00741-3 4 868 876 en 2020-T1-001-031 2017-T2-2-069 A19D9a0096 RG8/20 RG104/18 Nature Sustainability © 2021 The Author(s), under exclusive licence to Springer Nature Limited. All rights reserved. This paper was published in Nature Sustainability and is made available with permission of The Author(s). application/pdf |
| spellingShingle | Engineering::Materials::Energy materials Carbon Dioxide Catalysts Lv, Chade Zhong, Lixiang Liu, Hengjie Fang, Zhiwei Yan, Chunshuang Chen, Mengxin Kong, Yi Lee, Carmen Liu, Daobin Li, Shuzhou Liu, Jiawei Song, Li Chen, Gang Yan, Qingyu Yu, Guihua Selective electrocatalytic synthesis of urea with nitrate and carbon dioxide |
| title | Selective electrocatalytic synthesis of urea with nitrate and carbon dioxide |
| title_full | Selective electrocatalytic synthesis of urea with nitrate and carbon dioxide |
| title_fullStr | Selective electrocatalytic synthesis of urea with nitrate and carbon dioxide |
| title_full_unstemmed | Selective electrocatalytic synthesis of urea with nitrate and carbon dioxide |
| title_short | Selective electrocatalytic synthesis of urea with nitrate and carbon dioxide |
| title_sort | selective electrocatalytic synthesis of urea with nitrate and carbon dioxide |
| topic | Engineering::Materials::Energy materials Carbon Dioxide Catalysts |
| url | https://hdl.handle.net/10356/154705 |
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