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在ITO支持的亚纳米Pt集群上充分利用电催化的进化:由流动性Pt化物种控制的高,大小依赖的活动
Simran Kumari1, Tsugunosuke Masubuchi2, Henry S White2
1Chemical and Biomolecular Engineering Department, University of California, Los Angeles, California 90095, United States.
演化反应 (HER) 的电催化活性随着 (Pt) 集群大小在氧化物 (ITO) 上增加. 与散装相比,较小的Pt团形成化化合物,增强吸附和HER活性.
科学领域:
- 表面科学
- 电催化
- 计算化学
背景情况:
- (Pt) 集群是演化反应 (HER) 的关键电催化剂.
- 了解集群大小和应用潜力的Pt电催化活性对催化剂设计至关重要.
- 氧化物 (ITO) 作为电化学应用中的导电支材料.
研究的目的:
- 研究团大小 (n = 1,4,7,8) 对演化反应 (HER) 活性的影响.
- 检查应用电位和集群大小对吸附和电催化性能的影响.
- 在电化学条件下的相互作用时阐明Pt集群的结构和电子变化.
主要方法:
- 在ITO电极上使用原子尺寸选择的Pt集群进行组合实验研究.
- 使用密度函数理论 (DFT) 计算,包括全局优化和大规范方法.
- 分析了低潜能沉积 (HUPD) 及其与应用潜能和Pt集群大小的相关性.
主要成果:
- 对于孤立的Pt原子 (Pt1/ITO),HER的电催化活性是可以忽略不计的,但随着集群大小的增加而显著增加.
- 与多晶体Pt相比,Pt7/ITO和Pt8/ITO的活性大约是每个Pt原子的两倍.
- 在HER值潜力下,Pt集群 (n=4,7,8) 形成Pt化物化合物,相对于散装Pt,吸附的量是Pt的两倍.
结论:
- 团大小是决定HER电催化活性的一个关键因素.
- 形成Pt化物种显著增强了吸附和HER性能.
- 准确预测HER活性需要考虑能量可访问的Pt-化物结构和潜在依赖现象的组合.
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