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单原子催化剂的高吞吐量设计,具有非平面和三重-N协调,用于高效的H2O电合成

Jingjing Jia¹, Zhenxin Li¹, Zhiyuan Sang^1,2

¹Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and Engineering, Tianjin, University, Tianjin, 300072, China.

Angewandte Chemie (International ed. in English)

|December 31, 2024

概括

具有特定的金属协调性的非平面单原子催化剂 (SAC) 显示出增强的氧降解反应 (ORR) 活性. 一个新的描述符, Δεd-p,准确地预测了高效过氧化电合成的性能.

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:

非平面的单原子催化剂 (SAC) 提供独特的氧降解反应 (ORR) 能力,由于轨道从不对称的协调重新排列.
由于选配置和控制协调结构的困难,调查非平面SAC具有挑战性.

研究的目的:

开发和验证非平面SACs (ppy-MN3),其中金属原子由pyrrole-N三重协调,以获得高效的2e-ORR.
提出一种新的描述符 (Δεd-p) 基于电子结构来预测催化活动,以补充d波段中心理论.

主要方法:

结合高通量选和非平面SAC的实验验证 (ppy-MN3).
为了活动预测,利用了一个新的描述符,金属d-band中心和N-连接体p-band中心 (Δεd-p) 之间的能量差异.
在性条件下对2e-ORR活性和选择性的ppy-ZnN3的实验验证.

主要成果:

确定了ppy-ZnN3作为2e-ORR的高度活跃和选择性催化剂,具有较低的动力障碍.
在性条件下实现了高电催化H2O2产量 (43mol g-1h-1) 和选择性 (92%).
证明了 Δεd-p 描述符在将电子结构与催化性能相关联方面的有效性.

结论:

提出了以性能为导向的,用于高效的H2O2电合成的非平面SACs的精确协调设计的概念证明.
这项研究为d波段理论提供了重要的补充,用于预测电化学过程中非平面配置中的催化活性.

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