| 第一作者： | Chen, ZP (Chen, Zhipeng); Zhang, XX (Zhang, Xinxin); Liu, W (Liu, Wei); Jiao, MY (Jiao, Mingyang); Mou, KW (Mou, Kaiwen); Zhang, XP (Zhang, Xiangping); Liu, LC (Liu, Licheng); |
|---|---|
| 联系作者： | Chen, ZP (Chen, Zhipeng); Zhang, XX (Zhang, Xinxin); Liu, W (Liu, Wei); Jiao, MY (Jiao, Mingyang); Mou, KW (Mou, Kaiwen); Zhang, XP (Zhang, Xiangping); Liu, LC (Liu, Licheng); |
| 发表年度： | 2021 |
| 期： | 4 |
| 卷： | 14 |
| 页： | 2349-2356 |
| 摘要： | Although the Faraday efficiency (FE) for CO production of single-atom catalysts immobilized on nitrogen-doped carbon supports (M-N/C) for the CO2 electrocatalytic reduction reaction (CO2RR) is generally over 90%, M-N/C catalysts demonstrate a poor reaction current density, which is much worse than the current density at the industrial level. Herein, we first report a generalized amination strategy to significantly increase the current density for CO production of M-N/C catalysts (M = Ni, Fe, Zn). Among them, the aminated Ni single-atom catalyst achieves a remarkable CO partial current density of 450 mA cm(-2) (a total current density over 500 mA cm(-2)) with a nearly 90% CO FE at a moderate overpotential of 0.89 V, and particularly CO FE can be maintained over 85% in a wide operating potential range from -0.5 V to -1.0 V. DFT calculations and experimental research demonstrate that the superior activity is attributed to enhanced adsorption energies of CO2* and COOH* intermediates caused by the regulation of the electronic structure of the aminated catalysts. This work provides an ingenious method for significantly increasing the current density at the industrially-relevant level of single-atom catalysts for the CO2RR. |
| 刊物名称： | ENERGY & ENVIRONMENTAL SCIENCE |
| 影响因子： | 33.25 |
| 全文链接： | https://pubs.rsc.org/en/content/articlelanding/2021/EE/D0EE04052E |
