通过在局部对称性破碎的单原子催化剂上通过CO2减少对酸盐的连续电生成
Juncai Dong1, Yangyang Liu2,3, Jiajing Pei4
1Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China. dongjc@ihep.ac.cn.
Nature communications
|October 27, 2023
概括
用平面对称性破碎的CuN3单原子催化剂 (SAC) 进行了合成,以实现高效的电催化二氧化碳减排. 这种设计克服了与催化性质相关联的协调对称性的局限性,从而导致高格式选择性.
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:
- 原子级协调工程是单原子催化剂 (SAC) 的关键.
- 在SAC中,协调对称性和催化性质之间缺乏普遍的相关性.
- 合理的SAC设计需要理解结构-属性关系.
研究的目的:
- 为了合成平面对称性破碎的CuN3 (PSB-CuN3) SACs用于电催化 CO2 减少.
- 调查局部对称性破坏对催化性能的影响.
- 建立协调对称性和格式选择性之间的相关性.
主要方法:
- 平面对称性破碎的CuN3 SACs的微波加热合成.
- 在流电池中进行电催化二氧化碳减排测试.
- 操作X射线光谱学和用于结构和电子分析的理论计算.
主要成果:
- PSB-CuN3催化剂在 -0.73 V 与 RHE 之间实现了 94.3% 的形式选择性,优于对称 CuN4 催化剂.
- 在流细胞中,高格式选择性 (>90%) 在94.4mA cm-2维持了100小时.
- 对称性破坏诱导了dsp杂交,将催化活动与金属中心的微环境相关联.
结论:
- 在CuN3 SAC中打破平面D4h对称性可增强电催化CO2的减少以形成.
- 在局部对称性,协调环境和催化选择性之间建立了强烈的相关性.
- 这项工作为设计具有定制局部对称性的高效SAC提供了新的策略.
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