文献类型：期刊文献

英文题名：Quantifying Visible-Light-Induced Electron Transfer Properties of Single Dye-Sensitized ZnO Entity for Water Splitting

作者：Ma, Hui[1,2];Ma, Wei[1,2];Chen, Jian-Fu[3];Liu, Xiao-Yuan[1,2];Peng, Yue-Yi[1,2];Yang, Zhe-Yao[1,2];Tian, He[1,2];Long, Yi-Tao[1,2]

机构：[1]East China Univ Sci & Technol, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Res Inst Ind Catalysis & Ctr Computat Chem, Key Lab Adv Mat, Shanghai 200237, Peoples R China

年份：2018

卷号：140

期号：15

起止页码：5272

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20181605035309);WOS:【SCI-EXPANDED(收录号:WOS:000430642000051)】；

基金：This research was supported by the National Natural Science Foundation of China (21421004, 21327807, 21775043), the Program of Introducing Talents of Discipline to Universities (B16017), Innovation Program of Shanghai Municipal Education Commission (2017-01-07-00-02-E00023), and the Fundamental Research Funds for the Central Universities (222201718001, 222201717003).

语种：英文

外文关键词：Electrochemistry - Film thickness - II-VI semiconductors - Monte Carlo methods - Photocatalytic activity - Electron transport properties - Microelectrodes - Titanium dioxide

摘要：Quantifying the photoinduced electron transfer properties of a single entity is of paramount importance for darifying the link between the photoelectrochemical performance and the specific properties of an individual. Here, we successfully monitored the photoelectrochemical behavior of a single dye sensitized ZnO entity on a Au ultramicroelectrode with different TiO2 film thicknesses. Due to a trap-limited electron diffusion in TiO2 film, a sub-millisecond photocurrent transient was observed for an individual N719@ZnO associated with single-particle photo catalytic water splitting. Furthermore, a Monte Carlo random walk numerical simulation model was developed to simulate the photoinjected electron transport dynamics and recombination in a nanoparticulate TiO2 film. Our approach allowed the photocatalytic properties of N719 at the single-molecule to be quantified, and electron diffusivity and electron collection efficiency as a function of the film thickness were estimated by simulation analyses. Excellent agreement was obtained between the experimental results and theoretical simulations, indicating that the underlying photoinduced electron transfer processes can be reliably explored.