铟
甲醇
催化作用
兴奋剂
吸附
化学
Atom(片上系统)
工作职能
无机化学
材料科学
有机化学
物理化学
计算机科学
光电子学
电极
嵌入式系统
作者
Qin Chen,Qiang Ke,Xiuyun Zhao,Xin Chen
标识
DOI:10.1016/j.mcat.2023.113123
摘要
The doping of foreign metals can modify the electronic properties of the original catalyst surfaces, thereby changing the catalytic activity. Realistic surfaces possess many defects, such as step sites. Herein, the first-principles calculation is implemented to research how indium doping on stepped Rh(211) alters the catalytic activity for methanol synthesis. The calculated substitution energy shows that the indium atom tends to be doped at the step edge of Rh(211). Almost all species prefer to adsorb at the step-edge sites because the surface atoms at the step-edge possess the lowest coordination number. The electronic structure analysis demonstrates that the activation degree of CO2* chiefly relies on the charge transfer between CO2* and catalyst. Furthermore, the doped indium atoms make In/Rh(211) expose more H* adsorption sites and promote the relative stability of adsorbed species on In/Rh(211). Besides, the doping of indium significantly inhibits the generation of by-product CO*, and enables the activation barrier to be as low as 0.98 eV for the rate-determining step on In/Rh(211), which is much lower than that of some reported catalysts. The ultrahigh catalytic activity of In/Rh(211) might be attributed to the decrease of the work function induced by the doping of indium, enhancing the relative stability of reaction species and CO2* activation degree.
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