物理化学学报2025，Vol.41Issue(7)：85-94,10.DOI:10.1016/j.actphy.2025.100074
调节NNU-55(Fe)的d带中心以增强CO2吸附和光催化活性
Modulating the d-band center of NNU-55(Fe)for enhanced CO2 adsorption and photocatalytic activity
摘要
Abstract
Photocatalytic reduction of carbon dioxide(CO2)has emerged as an effective technology to transform CO2 into valuable chemicals.Metal-organic frameworks(MOFs)show great promise due to their adjustable structures,huge specific surface areas,excellent catalytic properties,and remarkable photo responsiveness.Herein,the MOF material NNU-55(Fe)was employed for the photocatalytic transformation of CO2 into carbon monoxide(CO).Through electronic modulation of the active metal center(Fe-N4)via inorganic anionic ligand tuning,the photocatalytic performance of NNU-55(Fe)MOFs can be easily regulated.Notably,NO-3-coordinated NNU-55(Fe)demonstrated superior catalytic performance compared to SO42--and Cl--coordinated catalysts,achieving a CO production of 124 μmol∙g-1 within 3 h.The stronger electron donation capacity of NO-3 leads to an improved electron density of Fe centers,which lowers the Fe d-band center and enhances the bonding orbital occupancy in the adsorption system,thereby increasing the adsorption strength of CO2 and reduction activity.This study highlights a simple strategy for altering the catalytic activity and electrical structure of MOFs by altering the coordinated inorganic ligands of metal sites,offering a novel approach to developing efficient photocatalytic materials.关键词
金属有机框架/配位结构/d带中心/CO2吸附/光还原Key words
MOFs/Coordination structure/d-band center/CO2 adsorption/Photoreduction分类
化学化工引用本文复制引用
杨雪琦,赵俊涛,叶家伟,周德森,狄廷敏,张军..调节NNU-55(Fe)的d带中心以增强CO2吸附和光催化活性[J].物理化学学报,2025,41(7):85-94,10.基金项目
This study was supported by the National Natural Science Foundation of China(NSFC)(22308341,22005228)and the Scientific Research Foundation of Wuhan Institute of Technology(K2024047).国家自然科学基金(22308341,22005228)和武汉工程大学科学研究基金(K2024047)资助项目 （NSFC）
