揭示单个原子催化物的活性结构:电荷容量和结合的关键作用
1Texas Materials Institute and Department of Mechanical Engineering, The University of Texas at Austin, Austin, Texas 78712, United States.
Journal of the American Chemical Society
|March 4, 2020
概括
一个原子催化剂显示出高电化学二氧化碳减排 (CO2R) 的活性. 新发现揭示了电荷容量和键是其催化起源和选择性的关键,
科学领域:
- 材料科学
- 电化学
- 催化剂
背景情况:
- 在石墨烯上的单原子催化剂对电化学CO2降解 (CO2R) 的活性很高.
- 精确的催化机制和最佳的协调结构仍然不清楚,之前的DFT计算表明不活性.
研究的目的:
- 阐明二氧化碳单原子催化剂的催化起源.
- 确定这些催化剂活动和选择性的关键因素.
主要方法:
- 使用*ab initio*分子动力学 (AIMD) 来评估反应动力障碍.
- 使用"缓慢增长"采样方法来评估催化性能.
- 嵌入式充电容量和结合效应,在以前的DFT研究中经常被忽视.
主要成果:
- 电荷容量和键显著影响催化活性和选择性.
- 高充电容量可以降低电化学屏障,从而实现更大的充电传输.
- 结合稳定了中间体并促进了质子转移,增强了CO2R对进化的选择性.
结论:
- 对Ni原子的混合协调环境 (1N,3C) 被确定为CO2R的最佳环境.
- 这项研究解决了关于基于Ni的单原子催化剂的长期难题.
- 强调充电能力和结对于设计水溶液中有效的电催化剂的重要性.
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