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通过从纳米集群中去除单个金属原子来构建原子级缺陷作为催化场所

Shuang Wang¹, Chao Han¹, Xing Chen¹

¹Institutes of Physical Science and Information Technology, Department of Chemistry and Centre for Atomic Engineering of Advanced Materials, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials, Anhui University, Hefei, Anhui 230601, China.

|June 30, 2025

概括

从Au₂₁星团中去除一个黄金原子,就产生了一个有缺陷的Au₂₀星团. 这个有缺陷的集群表现出电化学二氧化碳还原反应 (eCO₂RR) 的增强催化活性.

科学领域:

纳米材料科学科学纳米材料科学
催化剂是一种催化剂.
表面工程是什么?表面工程是什么?

背景情况:

黄金集群是有希望的催化剂,但它们的活动对结构修改很敏感.
了解结构-活动关系对于设计高效的催化剂至关重要.

研究的目的:

在黄金集群中设计单个原子缺陷.
为了研究这种缺陷对电化学二氧化碳减排中的催化性能的影响.

主要方法:

表面工程的Au₂₁(AdmS) ₁₃S(F₃Ph₃P) 创建的Au₂₀(AdmS) ₁₄(PhPy₂P). 在这个过程中,AU₂₀ (AU) 的表面工程是AU₂₁ (AU) 的表面工程,而AU₂₁ (AU) 的表面工程是AU₂₁ (AU) 的表面工程.
结构分析和Au₂₁和Au₂₀集群的比较.
对电化学二氧化碳还原反应 (eCO₂RR) 的两个集群的电催化评估.

主要成果:

删除第21个黄金原子暴露了核心中的第9个黄金原子,创建了一个催化活性站点.
缺陷的Au₂₀集群显示了比eCO₂RR.中原始的Au₂₁集群显著更高的催化活性.
Au₂₀在 -1.3 V 的电流密度是Au₂₁的3倍,CO (FE_CO) 的法拉代最大效率在 -0.9 V 的92.47%,而Au₂₁的53.66%.

结论:

引入原子级缺陷的表面工程是提高黄金集群催化力的有效策略.
缺陷的Au20星团中暴露的核心金原子是其改进的CO2吸附和减少的关键.
理论计算证实了活跃地点的增强电荷转移,促进了CO2的减少.

关键词:

活跃的网站活跃的网站在原子层面的缺陷.催化机制是一种催化机制.eCO2RRR 的使用情况.同类纳米集群的同类纳米集群.

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