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构建未和的Ru原子阵列被限制在Mn氧化物中,以促进中性降水

Qi Hu¹, Jianyong Cao¹, Shuai Qi¹

¹College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, Guangdong, People's Republic of China.

Angewandte Chemie (International ed. in English)

|September 23, 2024

概括

这项研究通过在Mn氧化物中创建有序的低协调的 (Ru) 原子阵列来增强中性演化反应 (HER). 这种设计可以促进水分和H*重组,性能优于商业Pt/C催化剂.

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 (Ru) 催化剂对酸演化反应 (HER) 具有很高的活性.
它们的中性HER活性受缓慢的水解离和中性电解质中的H*重组动力学限制.
开发高效的中性HER电催化剂对于可持续的生产至关重要.

研究的目的:

在Mn氧化物 (Li₄Mn₅O₁₂) 中限制下,设计和合成有序的低协调的Ru原子阵列.
增强水分离和H*重组,以改善中性HER活性.
在中性介质中研究基于Ru的电催化剂的结构-活性关系.

主要方法:

在Li₄Mn₅O₁₂.内有序的低坐标Ru原子数组的合成.
在中性电解质中的演化反应 (HER) 活动的电化学表征.
控制实验以阐明低协调的Ru原子和阵列结构的作用.
理论计算 (例如,DFT) 来理解反应机制.

主要成果:

与中性介质中的商业Pt/C相比,合成的Ru原子阵列在HER活动中表现出6倍的增强.
低协调的Ru原子通过与氧原子相互作用,促进了水的快速解离.
阵列结构允许通过Tafel路径直接进行H*-H*重组,与使用较慢的Heyrovsky路径的孤立原子不同.

结论:

在Mn氧化物中订购的低协调的Ru原子阵列显著提高了中性HER的性能.
控制Ru的协调环境和原子排列是提高电催化活性的关键.
这项工作提供了通过组装有序的金属原子来设计先进的电催化剂的新策略.

关键词:

协调结构协调结构金属原子数组的金属原子数组.金属的单个原子是一个金属原子.中性进化反应反应水的电解是水的电解.

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