增强*COOH吸附在富含Ni-N4位点上的有效的酸性CO2电解
Ziwen Mei1, Yingjie He2, Kang Liu1
1Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, School of Physics, Central South University, Changsha, Hunan 410083, China.
Journal of the American Chemical Society
|September 5, 2025
概括
具有丰富的Ni-N4位点的工程单原子催化剂提高了酸性CO2降解反应 (CO2RR) 的性能. 这一策略增强了中间结合,在工业相关的电流密度下实现了高的碳选择性和效率.
科学领域:
- 电化学和催化
- 材料科学
- 表面化学
背景情况:
- 由于高碳选择性,单原子 (Ni) 催化剂对酸性二氧化碳还原反应 (CO2RR) 是有前途的.
- 性能限制源于高电流密度与*COOH中间体的弱相互作用.
- 有效的二氧化碳转化需要更强的Ni-N4位点的中间结合.
研究的目的:
- 通过支持空位工程,在孤立的Ni-N4位点上增强*COOH吸附.
- 使用边缘丰富的Ni-N4位点在酸性介质中提高CO2RR活性和选择性.
- 研究电子结构调制以提高单原子催化剂的性能.
主要方法:
- 密度函数理论 (DFT) 计算用于电子结构和结合能分析.
- 偏差校正高角度环状暗场扫描传输电子显微镜 (HAADF-STEM) 用于位点特征.
- 用于验证的X射线吸附光谱 (XAS) 和现场减弱的全反射表面增强红外吸收光谱 (ATR-SEIRAS).
主要成果:
- 通过HAADF-STEM和XAS成功引入了富含Ni-N4的边缘部位.
- DFT计算显示Ni d带中心上升,加强*COOH结合.
- 优化催化剂在800 mA cm-2时实现了高于94.5%的CO法拉代效率,在pH1时达到44.2%的能量效率.
结论:
- 支持空缺工程,以创建富含Ni-N4的边缘,有效地增强*COOH吸附.
- 这种策略在高电流密度下显著提高了酸性CO2RR的活性和选择性.
- 边缘工程为优化工业应用的单原子催化剂提供了一种多功能途径.
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