Sequential co-reduction of nitrate and carbon dioxide enables selective urea electrosynthesis
© 2024. The Author(s)..
Despite the recent achievements in urea electrosynthesis from co-reduction of nitrogen wastes (such as NO3-) and CO2, the product selectivity remains fairly mediocre due to the competing nature of the two parallel reduction reactions. Here we report a catalyst design that affords high selectivity to urea by sequentially reducing NO3- and CO2 at a dynamic catalytic centre, which not only alleviates the competition issue but also facilitates C-N coupling. We exemplify this strategy on a nitrogen-doped carbon catalyst, where a spontaneous switch between NO3- and CO2 reduction paths is enabled by reversible hydrogenation on the nitrogen functional groups. A high urea yield rate of 596.1 µg mg-1 h-1 with a promising Faradaic efficiency of 62% is obtained. These findings, rationalized by in situ spectroscopic techniques and theoretical calculations, are rooted in the proton-involved dynamic catalyst evolution that mitigates overwhelming reduction of reactants and thereby minimizes the formation of side products.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2024 |
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| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:15 |
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| Enthalten in: |
Nature communications - 15(2024), 1 vom: 02. Jan., Seite 176 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Li, Yang [VerfasserIn] |
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| Anmerkungen: |
Date Revised 05.01.2024 published: Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1038/s41467-023-44131-z |
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NLM366584405 |
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| 520 | |a © 2024. The Author(s). | ||
| 520 | |a Despite the recent achievements in urea electrosynthesis from co-reduction of nitrogen wastes (such as NO3-) and CO2, the product selectivity remains fairly mediocre due to the competing nature of the two parallel reduction reactions. Here we report a catalyst design that affords high selectivity to urea by sequentially reducing NO3- and CO2 at a dynamic catalytic centre, which not only alleviates the competition issue but also facilitates C-N coupling. We exemplify this strategy on a nitrogen-doped carbon catalyst, where a spontaneous switch between NO3- and CO2 reduction paths is enabled by reversible hydrogenation on the nitrogen functional groups. A high urea yield rate of 596.1 µg mg-1 h-1 with a promising Faradaic efficiency of 62% is obtained. These findings, rationalized by in situ spectroscopic techniques and theoretical calculations, are rooted in the proton-involved dynamic catalyst evolution that mitigates overwhelming reduction of reactants and thereby minimizes the formation of side products | ||
| 650 | 4 | |a Journal Article | |
| 700 | 1 | |a Zheng, Shisheng |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Hao |e verfasserin |4 aut | |
| 700 | 1 | |a Xiong, Qi |e verfasserin |4 aut | |
| 700 | 1 | |a Yi, Haocong |e verfasserin |4 aut | |
| 700 | 1 | |a Yang, Haibin |e verfasserin |4 aut | |
| 700 | 1 | |a Mei, Zongwei |e verfasserin |4 aut | |
| 700 | 1 | |a Zhao, Qinghe |e verfasserin |4 aut | |
| 700 | 1 | |a Yin, Zu-Wei |e verfasserin |4 aut | |
| 700 | 1 | |a Huang, Ming |e verfasserin |4 aut | |
| 700 | 1 | |a Lin, Yuan |e verfasserin |4 aut | |
| 700 | 1 | |a Lai, Weihong |e verfasserin |4 aut | |
| 700 | 1 | |a Dou, Shi-Xue |e verfasserin |4 aut | |
| 700 | 1 | |a Pan, Feng |e verfasserin |4 aut | |
| 700 | 1 | |a Li, Shunning |e verfasserin |4 aut | |
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