煤炭转化2019，Vol.42Issue(3)：40-48,9.DOI:10.19726/j.cnki.ebcc.201903006
合成气和硫化氢气氛下Rh表面扩散的密度泛函理论研究
Effects of Syngas and H2S Atmosphere on Rh Surface Diffusion: a DFT Study
摘要
Abstract
To understand the sintering and improve the stability of Rh catalyst,the diffusion of Rh species on Rh(111) surface under CO,H2 and H2S atmospheres at different temperatures were investigated using density functional theory.Under CO and H2 atmosphere,as the temperature increases,the diffusivity of Rh-CO and Rh-H complex becomes faster than that of Rh adatom,which indicates that CO and H2 can accelerate Rh surface diffusion and promotes the sintering of Rh catalyst.In H2 S atmosphere,the negative formation free energies of Rh-S complexes indicate that Rh-S complexes are easy to form on Rh(111) surface.Compared with that of Rh species,Rh-CO and Rh-H complex,the diffusivity of RhS complex is very large at 10-6 level of H2S.Therefore,Rh catalyst is extremely sensitive to the S-containing species and has lower sulfur tolerance.关键词
Rh表面扩散/一氧化碳/氢气/硫化氢/密度泛函理论Key words
Rh surface diffusion/CO/H2/H2S/DFT分类
化学化工引用本文复制引用
郝晓斌,章日光,凌丽霞,王宝俊..合成气和硫化氢气氛下Rh表面扩散的密度泛函理论研究[J].煤炭转化,2019,42(3):40-48,9.基金项目
Project (21736007) Supported by the Key Projects of National Natural Science Foundation of China,Projects (21476155,21776193) Supported by the National Natural Science Fourdation of China. （21736007）
