燃料化学学报（中英文）2026，Vol.54Issue(6)：151-159,9.DOI:10.1016/S1872-5813(26)60643-3
Pt基负载型催化剂上不同CO吸附类型的原理探究
Principles of different CO adsorption types on Pt-based supported catalysts
摘要
Abstract
This study systematically investigated the CO adsorption behavior and electron transfer mechanism on Ptn/γ-Al2O3 catalysts using density functional theory(DFT)calculations.Combined with infrared vibrational spectroscopy(FT-IR),electron difference density(EDD)and charge decomposition analysis(CDA),the authors revealed how Pt cluster size regulated CO adsorption configuration,electron transfer,and C-O bond vibrational frequency.The results show that small Pt4 sub-nanometric clusters,due to their highly coordinated unsaturated Pt atoms,have strong d-electron feedback,resulting in full filling of CO's π* antibonding orbitals,a significant weakening of the C-O bond,and a redshift in the IR frequency.Large Pt13 sub-nanometric clusters,due to their dense structure,experience electron delocalization,weaken feedback,enhance C-O bonding,and have a blueshift in the IR frequency.The electron transfer intensity increases in linear,bridge,and multi-terminal adsorption,respectively.Bridge adsorption is most sensitive to size,with an IR blueshift of 81 cm-1 observed when the number of Pt atoms increases from 4 to 13.Multi-terminal adsorption exhibits a stable frequency due to a"saturation effect".This study establishes a comprehensive correlation among Pt size,electronic structure,adsorption properties,and infrared response,elucidating the CO adsorption mechanism on Pt-based catalysts and providing atomic-scale theoretical guidance for the design of efficient catalysts.关键词
Pt团簇尺寸/CO吸附/红外振动频率/电子转移/密度泛函理论Key words
Pt cluster size/CO adsorption/infrared vibrational frequency/electron transfer/density functional theory分类
化学化工引用本文复制引用
何凯,苏旭艳,曲壮,杨野,秦玉才,宋丽娟..Pt基负载型催化剂上不同CO吸附类型的原理探究[J].燃料化学学报（中英文）,2026,54(6):151-159,9.基金项目
Supported by National Natural Science Foundation of China(2023YFA1507700,U1908203),Liaoning Revitalization Talents Program(XLYC2203165),Natural Science Foundation of Liaoning Province(2024-BS-226),Basic Scientific Research Project of Liaoning Province Department of Education(JYTQN2023342).国家自然科学基金(2023YFA1507700,U1908203),辽宁省兴辽英才计划(XLYC2203165),辽宁省自然科学基金(2024-BS-226)和辽宁省教育厅高校基本科研项目(JYTQN2023342)资助 （2023YFA1507700,U1908203）
