化学
面(心理学)
电子转移
光催化
锐钛矿
电子
选择性
Atom(片上系统)
半导体
光化学
化学物理
催化作用
光电子学
材料科学
物理
有机化学
量子力学
社会心理学
五大性格特征
嵌入式系统
计算机科学
人格
心理学
作者
Hongru Zhou,Min Wang,Fangfang Kong,Zhiwei Chen,Zhaolin Dou,Feng Wang
摘要
The electron transfer (ET) from the conduction band of the semiconductor to surface-bound species is a key step in the photocatalytic reaction and strongly affects the reactivity and selectivity, while the effect of catalyst surface structure on this process has rarely been explored due to the lack of an effective method. Herein, we have developed a strategy to detect and measure surface electrons' transfer energy to the adsorbates and disclosed a facet-dependent electron transfer energy over anatase TiO2. The photogenerated electrons are shallowly confined in the five-coordinated Ti atom (Ti5c) on the surface of the (101) facet with a transfer energy below 1.0 eV, while deeply confined in the six-coordinated Ti atom (Ti6c) on the subsurface of the (001) facet with a transfer energy higher than 1.9 eV. The different electron trap states strongly affect the ET process, thus regulating the photocatalytic activity. Taking formic acid (FA) dehydration as the probe reaction, a shallow trap of photoexcited electrons on the (101) facet of anatase TiO2 favors the dehydration of FA to CO, while a deep trap of photoexcited electrons on the (001) facet makes FA stable. Based on this knowledge, we successfully controlled the selectivity in the photocatalytic oxidation of biopolyols via selectively exposing the facet of TiO2. Through controlling the (001)/(101) facet, a wide range of biopolyols can be selectively converted into FA or CO with a selectivity of up to 80%. The present work disclosed a facet-dependent electron transfer process and provides a new horizon to the design of photocatalytic systems.
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