光催化
激发态
Atom(片上系统)
化学物理
密度泛函理论
材料科学
光化学
电子结构
载流子
基质(水族馆)
超短脉冲
半导体
化学
光电子学
原子物理学
计算化学
催化作用
物理
光学
嵌入式系统
地质学
海洋学
生物化学
激光器
计算机科学
作者
Zhe Xu,Yimin Zhang,Ziyu Wang,Daqiang Chen,Peiwei You,Shunfang Li,Haizhong Guo,Sheng Meng
出处
期刊:Nano Letters
[American Chemical Society]
日期:2023-04-27
卷期号:23 (9): 4023-4031
被引量:1
标识
DOI:10.1021/acs.nanolett.3c00810
摘要
With the introduction of single atoms in photocatalysis, a small change in the electronic and geometric structure of the substrate can result in higher energy conversion efficiency, whereas the underlying microscopic dynamics are rarely illustrated. Here, employing real-time time-dependent density functional theory, we explore the ultrafast electronic and structural dynamics of single-atom photocatalysts (SAPCs) in water splitting at the microscopic scale. The results demonstrate that a single-atom Pt loaded on graphitic carbon nitride greatly promotes photogenerated carriers compared to traditional photocatalysts, and effectively separates the excited electrons from holes, prolonging the lifetime of the excited carriers. The flexible oxidation state (Pt2+, Pt0, or Pt3+) renders the single atom as an active site to adsorb the reactant and to catalyze the reactions as a charge transfer bridge at different stages during the photoreaction process. Our results offer deep insights into the single-atom photocatalytic reactions and benefit the design of high-efficiency SAPCs.
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