可再生能源2024，Vol.42Issue(4)：440-447,8.
焦油组分重整过程中关键反应的机理研究
Mechanism investigation of key reactions during tar component reforming process
摘要
Abstract
Density functional theory calculations were employed to investigate the mechanisms and energy changes involved in C-C bond cracking,CH4 reforming,and water gas shift reactions in the tar reforming process.The findings reveal that,in the C-C bond cracking reaction,C3H8 initially adsorbs onto the catalyst surface to form adsorbed C3H8*,subsequently undergoing cleavage to produce CH3*and CH2CH3*.While the cracking reaction is exothermic,it is hindered by a significant energy barrier and difficult to carry out.In the CH4 reforming reaction,CH4*undergoes sequential dehydrogenation reactions,producing CH3*,CH2*,and CH*.Comparatively,CH*has a greater tendency to react with OH* to form CHO*,which further undergoes dehydrogenation to form CO*.Additionally,H*generated in each step combines to form H2*.Throughout the CH4 reforming process,the rate-limiting step is the cracking of CH2*to CH*.In the water gas shift reaction,the OH*species formed from H2O*decomposition prefers to combine with CO*to generate COOH*rather than directly reacting with H*to produce H2*.COOH*removes H and generates COO*,which is the rate limiting step.关键词
焦油/重整/密度泛函理论/基元反应Key words
tar/reforming/density functional theory/elementary reaction分类
能源科技引用本文复制引用
杜文亚,于震宇,郭锐,孙超,邵正日,谢华清..焦油组分重整过程中关键反应的机理研究[J].可再生能源,2024,42(4):440-447,8.基金项目
辽宁省储能与能源利用技术重点实验室基金项目(CNWK202305). （CNWK202305）
