期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 121, 期 29, 页码 15665-15674出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.7b02424
关键词
-
资金
- NSF Graduate Research Fellowship Program
- NSF [CHE-1464804]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1464804] Funding Source: National Science Foundation
computational screens for oxygen evolution reaction (OER) catalysts based on Sabatier analysis have seen great success in recent years; however, the concept of using chemical descriptors to form a reaction coordinate has not been put under scrutiny for complex systems. In this paper, we examine critically the use of chemical descriptors as a method for conducting catalytic screens. Applying density functional theory calculations to a two-center metal oxide model system, we show that the Sabatier analysis is quite successful for predicting activities and capturing the chemical periodic trends expected for the first-row transition metal series, independent of the proposed mechanism. We then extend this analysis to heterodimer metallic systems-metal oxide catalysts with two different catalytically active metal centers-and find signs that the Sabatier analysis may not hold for these more complex systems. By performing a principal component analysis on the computed redox potentials, we show. (1) that a single chemical descriptor inadequately describes heterodimer overpotentials and (2) mixed metal overpotentials cannot be predicted using only pure-metal redox potentials. We believe that the analysis presented in this article shows a need to move beyond the simple chemical descriptor picture when studying more complex mixed metal oxide OER catalysts.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据