低碳化学与化工2025，Vol.50Issue(12)：21-29,9.DOI:10.12434/j.issn.2097-2547.20250074
基于密度泛函理论的异质结CoCu(100)/(111)表面催化合成气直接制乙醇机理研究
Mechanisms of direct synthesis of ethanol from syngas catalyzed by heterojunction CoCu(100)/(111)surface based on density functional theory
摘要
Abstract
As an emerging new energy technology,the direct synthesis of ethanol from syngas still faces problems such as low catalytic efficiency of catalysts and product selectivities.These problems are mainly due to the high energy barriers of C—O bond breakage and C—C bond formation,as well as the difficulty of controlling reaction.So,the reaction mechanisms of direct synthesis of ethanol from syngas on CoCu(100),CoCu(111)and heterojunction CoCu(100)/(111)surfaces were systematically studied by density functional theory(DFT),and the effects of heterojunction CoCu(100)/(111)on CO activation,C—O bond breakage and C—C bond formation were emphatically discussed.The results show that CO is hydrogenated at the Co site to generate CHO,further dissociated and hydrogenated to generate intermediate CHx,and CO is then inserted into intermediate CHx to generate intermediate CHxCO,and finally converted to ethanol by continuous hydrogenation.Compared with CoCu(100)and CoCu(111)surfaces,heterojunction CoCu(100)/(111)surface has advantages in promoting CO activation,C—O bond breakage and C—C bond formation due to its good local electronic structure.The results can provide an important theoretical basis for the design and optimization of high-efficiency Cu-based catalysts,and provide reference for the industrial application of synthesis of ethanol from syngas.关键词
催化机理/密度泛函理论/异质结CoCu(100)/(111)表面/局部电子结构优化Key words
catalytic mechanism/density functional theory/heterojunction CoCu(100)/(111)surface/local electronic structure optimization分类
能源科技引用本文复制引用
杜鹏龙,孟园园,王俊文,丁传敏,王莲,李刚森,段东红..基于密度泛函理论的异质结CoCu(100)/(111)表面催化合成气直接制乙醇机理研究[J].低碳化学与化工,2025,50(12):21-29,9.基金项目
国家自然科学基金(21978189,22308244) （21978189,22308244）
山西省自然基金面上项目(202203021221091). （202203021221091）
