对于单原子催化剂的通用协调工程策略,以实现高效的过氧化电合成.
Wei Liu1, Rui Chen1, Zhiyuan Sang1
1Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and Engineering, Tianjin University, Tianjin, 300072, P. R. China.
本研究引入了一种设计非贵金属单原子催化剂 (M-SACs) 的新策略,通过两电子氧降解反应 (2e-ORR) 有效地产生过氧化 (H2O2). 这种新的方法提高了H2O2电合成的催化剂性能和选择性.
科学领域:
- 电化学 电化学 电化学
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
背景情况:
- 非贵金属单原子催化剂 (M-SACs) 对于高效的两电子氧降解反应 (2e-ORR) 是至关重要的.
- M-SACs的协调配置显著影响过氧化 (H2O2) 电合成中的活性和选择性.
- 缺乏合理设计具有优化催化能力的M-SAC的通用策略.
研究的目的:
- 为M-SACs提出一个通用的协调工程策略,通过2e-ORR.针对H2O2电合成.
- 通过将异原子引入金属-N4协调球来定制中间体的电子结构和吸附强度.
- 为了优化M-SACs对2e-ORR的电催化性能.
主要方法:
- 通过将异原子 (O或S) 引入M-SACs的第一个协调球体,开发一个通用的协调工程策略.
- 合成 (O,N) 协调的 Co SAC (Co-N3O) 和 (S,N) 协调的 Ni SAC (Ni-N3S).
- 在性条件下评估2e-ORR活性,选择性和合成催化剂的稳定性.
- 进行理论动力学模拟以确认2e-ORR路径.
主要成果:
- 合成的Co-N3O和Ni-N3S催化剂表现出优异的2e-ORR活性 (发病潜力≈0.80V与RHE) 和选择性 (≈90%).
- 取得了高的H2O2产率,Co-N3O的14.2 mol g-1 h-1和Ni-N3S的17.5 mol g-1 h-1的H2O2产率.
- 两个催化剂的长期稳定性超过12小时.
- 理论模拟证实了有利的2e-ORR路径.
结论:
- 拟议的通用协调工程战略有效地优化了M-SAC用于2e-ORR.
- 在金属-N4位点中纳入异构原子可增强H2O2电合成的催化活性和选择性.
- 合成的Co-N3O和Ni-N3S催化剂为高效和选择性的H2O2生产提供了有希望的替代品.
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