Cu基催化剂上糠醛转化为糠醇结构敏感性的理论研究  

The structure-sensitive of Cu catalyst for furfural conversion to furfuryl alcohol:A theoretical study

作　　者：王贵儒 智翠梅[1] 杨雯[2] WANG Gui-ru;ZHI Cui-mei;YANG Wen(College of Chemical and Biological Engineering,Shanxi Key Laboratory of High Value Utilization of Coal Gangue,Taiyuan University of Science and Technology,Taiyuan 030024,China;Shanxi Key Laboratory of Metal Forming Theory and Technology,School of Material Science and Engineering,Taiyuan University of Science and Technology,Taiyuan 030024,China)

机构地区：[1]太原科技大学化学与生物工程学院煤矸石高值利用山西省重点实验室,山西太原030024 [2]太原科技大学材料科学与工程学院金属材料成形理论与技术山西省重点实验室,山西太原030024

出　　处：《燃料化学学报（中英文）》2023年第2期263-272,共10页Journal of Fuel Chemistry and Technology

基　　金：Shanxi Province Science Foundation for Youths(20210302124057);Doctoral Scientific Research Foundation of Taiyuan University of Science and Technology(2019060);Scientific and Technological Innovation Project of Colleges and Universities in Shanxi Province(2020L0353);Outstanding Doctoral Award Fund in Shanxi Province(20202017);National Natural Science fund of China(51871158).

摘　　要：本研究采用密度泛函理论方法以Cu(111)和Cu(211)表面为代表研究了Cu基催化剂上糠醛加氢转化为糠醇反应的结构敏感性。通过研究糠醛转化为糠醇过程中反应物、中间物种和产物的吸附及可能的反应机理,得出,在Cu(111)和Cu(211)表面上,糠醛C=O基团的碳原子首先加氢(F-CHO+H→F-CH_(2)O),然后氧原子加氢(F-CH_(2)O+H→F-CH_(2)OH),且第二步是整个反应的速率控制步骤。计算结果表明,Cu(211)表面对糠醇的生成具有较好的催化活性,这是由于该表面能够促进H_(2)解离和增强糠醛吸附,进而促进将糠醛转化为糠醇。本工作为通过调节金属催化剂的微观结构来控制生物质分子转化的活性和选择性提供了一种可行的方法。The structure-sensitive of Cu catalyst for furfural hydrogenation to furfuryl alcohol was explored by employing Cu(111)and Cu(211)model systems.Herein,the adsorption behavior of reactants and intermediates,and the possible reaction mechanism of furfuryl alcohol formation were investigated.For furfuryl alcohol formation,the preferred pathway is F-CHO+2H→F-CH_(2)O+H→F-CH_(2)OH,in which the second H addition is the rate-determining step.Meanwhile,Cu(211)surface exhibits higher activity to furfuryl alcohol formation than that on Cu(111)surface.According to our analysis,the undercoordinated sites on the Cu(211)surface could facilitate H_(2)dissociation and stabilize the adsorbed furfural,thereby promoting the furfural hydrogenation and the furfuryl alcohol formation.This work provides a feasible approach for regulating the catalytic activity and selectivity in furfural conversion.

关 键 词：Cu基催化剂 结构敏感性 糠醛加氢 糠醇 

分 类 号：TQ530[化学工程—煤化学工程]