石墨烯限域Fe2C活化CO的应变效应的理论研究
Theoretical study of the strain effects on CO activation by Fe2C confined with graphene
朱家亮 1李哲 1张煜华 1黎永秀 1李金林1
作者信息
- 1. 催化转化与能源材料化学教育部重点实验室,催化与材料科学湖北省重点实验室,中南民族大学,湖北武汉 430074
- 折叠
摘要
石墨烯限域碳化铁界面本征应变在催化费-托合成中具有重要作用.本文选择石墨烯限域Fe2C(121)表面模型,对Fe2C@graphene催化一氧化碳(CO)吸附和解离进行理论计算,考察其双轴应变效应.通过在±5％的范围内改变晶格应变,发现对于Fe2C位点的CO直接和氢助解离,表观能垒(Ea,app)和吸附能(Ead)呈非线性相关,对于石墨烯位点的CO直接和氢助解离,两者呈正常的Brønsted-Evans-Polanyi线性相关.该非线性相关性可通过分析吸附态和过渡态的限域间距的应变效应进行解释.本研究有助于深入理解Fe2C@graphene界面双轴应变在CO吸附活化过程中的本质作用.
Abstract
The intrinsic strains at the confinement interface of iron carbide with graphene play important roles in the catalytic Fischer-Tropsch synthesis.In this study,we performed theoretical study of the biaxi-al strain effects on the CO adsorption and dissociation on the Fe2C(121)surface covered by graphene(Fe2C@graphene).By varying the lattice strains within a range of±5％,the apparent energy barriers(Ea,app)correlate with the adsorption energies(Ead)in nonlinear scaling relations for the direct and H-as-sisted CO dissociation at the Fe2C active sites,which is normal Brønsted-Evans-Polanyi relation for those at the graphene sites.The nonlinear scaling relations can be interpreted by the strain effects on the con-finement distances in the adsorption and transition states.This study provides a deep understanding of the intrinsic strain effects of Fe2C@graphene for CO activation.
关键词
应变效应/碳化铁/限域效应/石墨烯/费-托合成Key words
strain effect/iron carbide/confinement effect/graphene/Fischer-Tropsch synthesis引用本文复制引用
基金项目
National Natural Science Foundation of China(21972170)
National Natural Science Foundation of China(22072184)
Fund for Academic Innovation Teams of South-Central Minzu University(XTZ24013)
出版年
2024
NETL
NSTL
万方数据