通过异原子调节单原子Ni中心的电子密度,以实现高效的CO2电还原
Yang Chen1,2, Xiaoli Pan1, Lin Li1
1CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
Small (Weinheim an der Bergstrasse, Germany)
|January 24, 2025
概括
用定制单原子催化剂可以提高电化学二氧化碳的减少. 这种修改通过优化中心的电子结构以实现高效的二氧化碳转换来提高性能.
科学领域:
- 材料科学 材料科学 材料科学
- 电化学 电化学 电化学
- 催化剂是一种催化剂.
背景情况:
- 单原子催化剂 (SAC) 为化学反应提供独特的特性.
- 控制SAC中的金属中心的电子结构对于增强催化活性至关重要.
- 电化学二氧化碳减排 (CO2RR) 是可持续能源解决方案的关键过程.
研究的目的:
- 系统地定制Ni1-NC SAC中Ni中心的电子结构.
- 为了研究加入富含电子的或缺乏电子的对CO2RR性能的影响.
- 为了建立电子结构和催化效率之间的定量关系.
主要方法:
- 合成Ni1-NC,Ni1-PNC和Ni1-BNC的单原子催化剂.
- 电化学表征,包括电流密度和法拉第效率测量.
- 密度函数理论 (DFT) 的计算和详细表征.
主要成果:
- 具有Ni1-N3P位点的Ni1-PNC催化剂表现出卓越的CO2RR性能.
- 实现了14.6mA cm-2的电流密度和90.6%的法拉第效率,用于在-0.8V与RHE相比的CO生产.
- 确定了Ni的价值状态和CO2RR性能之间的线性相关性.
- 合并将电子定位在Ni1中心,增强CO2吸附和*COOH中间体的形成.
结论:
- 的加入是调节单原子催化剂电子结构的有效策略.
- Ni1-PNC催化剂显示出有效的电化学二氧化碳减排的巨大潜力.
- 本研究提供了一种定量方法,用于设计高性能单原子催化剂.
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