Sequential co-reduction of nitrate and carbon dioxide enables selective urea electrosynthesis
書誌事項
- 公開日
- 2024-01-02
- 権利情報
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- https://creativecommons.org/licenses/by/4.0
- https://creativecommons.org/licenses/by/4.0
- DOI
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- 10.1038/s41467-023-44131-z
- 公開者
- Springer Science and Business Media LLC
説明
<jats:title>Abstract</jats:title><jats:p>Despite the recent achievements in urea electrosynthesis from co-reduction of nitrogen wastes (such as NO<jats:sub>3</jats:sub><jats:sup>−</jats:sup>) and CO<jats:sub>2</jats:sub>, 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 NO<jats:sub>3</jats:sub><jats:sup>−</jats:sup> and CO<jats:sub>2</jats:sub> 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 NO<jats:sub>3</jats:sub><jats:sup>−</jats:sup> and CO<jats:sub>2</jats:sub> reduction paths is enabled by reversible hydrogenation on the nitrogen functional groups. A high urea yield rate of 596.1 µg mg<jats:sup>−1</jats:sup> h<jats:sup>−1</jats:sup> 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.</jats:p>
収録刊行物
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- Nature Communications
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Nature Communications 15 (1), 176-, 2024-01-02
Springer Science and Business Media LLC
