金红石
光催化
瓶颈
障碍物
二氧化钛
氧气
析氧
分解水
激进的
材料科学
化学工程
化学物理
计算机科学
纳米技术
化学
政治学
工程类
物理化学
嵌入式系统
电极
催化作用
有机化学
冶金
法学
生物化学
电化学
作者
Dong Wang,Tian Sheng,Jianfu Chen,Haifeng Wang,P. Hu
出处
期刊:Nature Catalysis
[Springer Nature]
日期:2018-04-16
卷期号:1 (4): 291-299
被引量:215
标识
DOI:10.1038/s41929-018-0055-z
摘要
As the bottleneck in photocatalytic water splitting, the oxygen evolution reaction (OER) has drawn huge attention, but its efficiency still falls short of expectations. A widely accepted speculation is that the catalysts’ activity is insufficient (high reaction barriers need to be overcome). Here, we develop a first-principles method to investigate the photocatalytic OER at the water/TiO2(110) interface. A full mechanism uncovering the importance of radicals is determined. Kinetic analysis further enables to quantitatively estimate each possible obstacle in the process. We demonstrate unambiguously that the rate-determining factor of the OER varies with the concentration of surface-reaching photoholes (Ch+). Under experimental conditions, the intrinsic catalytic activity of TiO2(110) does not represent the main obstacle, but all steps involving the photoholes are slow due to their low concentrations. This suggests that the key to enhance the OER efficiency is to increase Ch+ before Ch+ reaches the estimated threshold (Ch+ = ~10−4). A high reaction barrier is often assumed as the limiting factor in photocatalytic oxygen evolution reactions on titanium dioxide. Now, it is shown that the hole concentration at the semiconductor’s surface is the actual bottleneck in determining the catalytic efficiency.
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