@article{Wang2024, 
author = {Shan-Fei Wang and Yangyang Li and Haiyan Wang and Jin-Xia Liang and Chun Zhu and Botao Qiao},
title = {Theoretical and experimental investigations on single-atom catalysis: Pt1/FeOx for water–gas shift reaction},
year = {2024},
journal = {Nano Research},
volume = {17},
number = {9},
pages = {8627-8637},
keywords = {density functional theory (DFT), thermocatalysis, single-atom catalyst (SAC), water–gas shift (WGS) reaction},
url = {https://www.sciopen.com/article/10.1007/s12274-024-6655-9},
doi = {10.1007/s12274-024-6655-9},
abstract = {Oxide-supported metal single-atom catalysts (SACs) have exhibited excellent catalytic performance for water–gas shift (WGS) reaction. Here, we report the single-atom catalyst Pt1/FeOx exhibits excellent medium temperature catalytic performance for WGS reactions by the density functional theory (DFT) calculations and experimental results. The calculations indicate that H2O molecules are easily dissociated at oxygen vacancies, and the formed *OH and *O are adsorbed on Pt1 single atoms and the adjacent O atoms, respectively. After studying four possible reaction mechanisms, it is found that the optimal WGS reaction pathway is proceeded along the carboxyl mechanism (pathway III), in which the formation of *COOH intermediates can promote the stability of Pt1/FeOx SAC and the easier occurrence of WGS reaction. The energy barrier of the rate-determining step during the entire reaction cycle is only 1.16 eV, showing the high activity for the medium temperature WGS reaction on Pt1/FeOx SAC, which was verified by experimental results. Moreover, the calculated turnover frequencies (TOFs) of CO2 and H2 formation on Pt1/FeOx at 610 K (337 °C) can reach up to 1.14 × 10−3 s−1·site−1 through carboxyl mechanism. In this work, we further expand the application potential of Pt1/FeOx SAC in WGS reaction.}
}