在单原子电催化剂中调节第二次超越的协调结构,以确认促进氨合成
Qinglin Li1, Lin Luo1,2, Xiangyang Guo1
1State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
Journal of the American Chemical Society
|January 15, 2025
概括
这项研究表明,单原子催化剂的二次协调球之外的结构显著影响了氨合成. 修改这种远程结构可增强催化活性,并可用于可充电电池.
科学领域:
- 材料科学
- 催化剂
- 电化学
背景情况:
- 微环境对单原子催化剂 (SAC) 的影响已知,但二次协调之外的结构的影响尚不清楚.
- 了解长距离结构效应对于优化SAC性能至关重要.
研究的目的:
- 调查二级协调球之外的远程结构对SAC电催化性能的影响.
- 探索可调节的协调球在酸盐合成中的作用.
主要方法:
- 合成金属有机框架 (MOF) 作为模型SAC (Cu12-NDI-X,X = NMe2,H,F) 具有定义的次要协调范围.
- 氨合成活性,产量和法拉第效率的电催化评估.
- 电化学分析以了解性能增强的机制.
主要成果:
- 在二次协调范围之外的远程功能组置换显著影响氨合成活动.
- 与其他修改相比,Cu12-NND-H显示出更高的氨产量 (35.1 mg·h−1·mgcat−1) 和法拉第效率 (98.7%).
- 这种增强的性能归因于Cu活性位点的可调 d 带中心,促进酸盐吸附和中间质子.
- 在Cu12-NND-H电极上,可以组装具有34.0mW·cm-2功率密度的可充电酸电池.
结论:
- 长距离的SAC结构调节是一种可行的策略,用于增强氨合成的催化活性.
- 通过在直接协调环境之外调整结构,这些发现为设计先进的SAC开辟了新的途径.
- 开发的催化剂对能源转换和储存应用,特别是可充电电池具有前景.
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