Cu单原子修饰对Fe(111)表面CO吸附性能及电子性质调变的第一性原理研究  

First-principles study on the CO adsorption and electronic properties of Fe(111) modified by Cu single atom

作　　者：孟宇 刘小艳[1] 白苗苗 王英 马亚军 曹直[2] MENG Yu;LIU Xiao-yan;BAI Miao-miao;WANG Ying;MA Ya-jun;CAO Zhi(Shaanxi Key Laboratory of Low Metamorphic Coal Clean Utilization,Yulin University,Yulin 719000,China;State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China)

机构地区：[1]榆林学院陕西省低变质煤洁净利用重点实验室,陕西榆林719000 [2]中国科学院山西煤炭化学研究所煤转化国家重点实验室,山西太原030001

出　　处：《燃料化学学报》2020年第4期440-447,I0004,共9页Journal of Fuel Chemistry and Technology

基　　金：陕西省自然科学基础研究计划项目(2019JQ-905,2018JZ2004);陕西省教育厅科研计划项目(19JS071);榆林市2019年科技计划项目(2019-83-1);榆林学院博士科研启动基金(17GK12,17GK13);煤转化国家重点实验室开放课题基金(J20-21-908)资助。

摘　　要：采用密度泛函理论方法研究了Cu单原子修饰对Fe(111)表面CO吸附性能和电子性质的调变作用,其中,Cu单原子修饰研究了吸附和取代两种方式。结果表明,CO在Cu修饰的Fe(111)面吸附能力都会变弱,一是Cu原子自身提供的位点对CO的吸附较弱;二是Cu会使其附近的Fe对CO的吸附变弱。分析电子性质表明,Cu作用于Fe表面后,会导致Cu附近Fe原子部分电子向Cu原子转移,进而削弱了Fe与吸附分子间电子交互作用而改变Fe原子的吸附能力。故Cu原子改性Fe表面可以很好地调变CO的吸附、解离及后续反应催化活性,这为进一步探究Cu改性Fe表面的合成气催化反应机理提供了基础信息。In this paper, the effect of Cu single atom modification on the adsorption of CO and electronic properties of Fe(111) surface has been studied by density functional theory(DFT). Two ways of adsorption and substitution have been studied for Cu mono-atom modification. The results show that the adsorption capacity of CO on the Cu modified Fe(111) becomes weak. One reason is that the sites provided by the Cu atom itself are weak for CO, and the other is that Cu weakens the adsorption of CO on the Fe nearby Cu. The analysis of electronic properties indicates that when Cu acts on the Fe(111), the part electrons of Fe can be transferred to the Cu, which weakens the electronic interaction between Fe and adsorbed molecules, and adjusts its adsorption capacity. Therefore, the Fe surface modified by Cu atom can well adjust the adsorption, dissociation and subsequent reaction catalytic activity of CO, which provides basic information to further explore the syngas catalytic reaction mechanism of Cu modified Fe surface.

关 键 词：Fe(111) 密度泛函理论 单原子Cu修饰 CO吸附 

分 类 号：O643.32[理学—物理化学]