硫掺杂铁基单原子催化剂结构与催化活性的密度泛函理论研究  

Density Functional Theory Study on the Structure and Catalytic Activity of Sulfur-Doped Iron-Based Single-Atom Catalysts

作　　者：蔺何[1] 张禹 刘晨帆 蔡璇璇 LIN He;ZHANG Yu;LIU Chenfan;CAI Xuanxuan(State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources,School of Chemistry,Xinjiang University,Urumqi Xinjiang 830017,China)

机构地区：[1]新疆大学化学学院省部共建碳基能源资源化学与利用国家重点实验室,新疆乌鲁木齐830017

出　　处：《新疆大学学报（自然科学版中英文）》2024年第2期228-235,共8页Journal of Xinjiang University(Natural Science Edition in Chinese and English)

基　　金：国家自然科学基金“锌离子电池正极材料的数据驱动高通量筛选研究”(22065032);固体表面物理化学国家重点实验室(厦门大学)开放课题“锌离子电池二维层状正极材料的高通量筛选及性能研究”(2020X32)。

摘　　要：通过密度泛函理论计算研究了硫原子掺杂对铁基单原子催化剂结构稳定性和催化活性的影响.采用结构优化和自由能计算的方法,评估了硫掺杂构型的热力学和电化学稳定性.结果表明:硫原子呈卫星式排布环绕单原子催化剂活性位点,形成稳定的催化剂结构,并对活性位点的电子结构进行调控.进一步比较了硫掺杂前后的催化活性,结果显示硫掺杂能够显著降低氧还原反应的过电势,特别是对称性破缺的体系表现出最低的过电势.The impact of sulfur(S)atoms doping on the structural stability and catalytic activity of iron-based single-atom catalysts was investigated using density functional theory calculations.Structural optimization and free energy calculations were employed to assess the thermodynamic and electrochemical stability of the S-doped configurations.The results demonstrated that S atoms adopted a satellite-like arrangement surrounding the active sites of the single-atom catalyst,leading to a stable catalyst structure and modulation of the electronic structure of the active sites.Furthermore,a comparison was made between the catalytic activities of the pristine catalyst and the S-doped catalysts,revealing a significant reduction in the overpotential of the oxygen reduction reaction upon S doping,particularly in systems with broken symmetry.

关 键 词：铁基单原子催化剂 密度泛函理论 氧还原 硫掺杂 

分 类 号：O643.3[理学—物理化学]