石墨烯负载单原子Pt吸附甲醛的理论计算  

Theoretical calculation on the adsorption of formaldehyde on graphene supported single atom Pt

作　　者：孙晓颖 卢健卓 赵震 SUN Xiaoying;LU Jianzhuo;ZHAO Zhen(College of Chemistry and Chemical Engineering,Shenyang Normal University,Shenyang 110034,China;State Key Laboratory of Heavy Oil Processing,China University of Petroleum,Beijing 102249,China)

机构地区：[1]沈阳师范大学化学化工学院,沈阳110034 [2]中国石油大学(北京)重质油国家重点实验室,北京102249

出　　处：《沈阳师范大学学报（自然科学版）》2024年第2期97-103,共7页Journal of Shenyang Normal University:Natural Science Edition

基　　金：国家自然科学基金资助项目(22172100,91845201)。

摘　　要：采用密度泛函理论方法研究石墨烯载体调变单原子Pt催化剂的几何结构、电子结构和吸附甲醛分子的性能.计算结果表明,单空穴位石墨烯负载的单原子Pt催化剂(Pt/GrGvac)电荷由Pt向载体转移,Pt带正电荷;杂原子B掺杂的单空穴位石墨烯负载的单原子Pt催化剂(Pt/3BGrGvac)电荷由载体向Pt转移,Pt带负电荷;杂原子N掺杂的单空穴位石墨烯负载的单原子Pt催化剂(Pt/3NGrGvac)中Pt带正电荷.不同石墨烯载体调变的单原子Pt催化剂均可吸附活化甲醛分子,电荷由单原子Pt催化剂向甲醛分子中的C原子转移.计算结果揭示Pt/3NGrGvac催化剂中Pt带正电荷更有利于甲醛分子的吸附活化.研究结果可为设计吸附甲醛的高效单原子催化剂提供理论基础.Density functional theory calculations were employed to study the geometric structure,electronic structure and properties of formaldehyde molecule adsorbed on single atom Pt catalyst.The calculation results showed that the charge of the single Pt atom at the mono-vacancy on graphene(Pt/Gr-vac)is transferred from Pt to support,hence Pt is positively charged.Conversely,the charge is transferred from support to Pt for boron doped graphene(Pt/3BGr-vac),and Pt is negatively charged.Interestingly,Pt is also positively charged on nitrogen doped graphene(Pt/3NGr-vac).The single Pt atom catalysts modified by different graphene supports can adsorb and activate formaldehyde molecules,and the charge is transferred from the Pt catalyst to the C atom in the formaldehyde molecule.The calculation results reveal that Pt is positively charged for the Pt/3NGr-vac catalyst,which is more conducive to the adsorption and activation of formaldehyde molecules.It provides a theoretical basis for the design of efficient single-atom catalysts for adsorbing formaldehyde.

关 键 词：石墨烯载体 单原子Pt催化剂 甲醛吸附 密度泛函理论 

分 类 号：O643.3[理学—物理化学]