Towards the selectivity distinction of phenol hydrogenation on noble metal catalysts  

作　　者：Shanjun Mao Zhe Wang Zhirong Chen Kejun Wu Kaichao Zhang Qichuan Li Huihuan Yan Guofeng Lü Guodong Huang Yong Wang 

机构地区：[1]Advanced Materials and Catalysis Group,Institute of Catalysis,Department of Chemistry,Zhejiang University,Hangzhou,310028,PR China [2]College of Chemical and Biological Engineering,Zhejiang University,Hangzhou,310027,PR China [3]Zhejiang NHU Company Ltd,Xinchang County,Zhejiang Province,PR China

出　　处：《Nano Materials Science》2023年第1期91-100,共10页纳米材料科学（英文版）

基　　金：This work was supported by Financial support from the National Natural Science Foundation of China(21908189,21872121);the National Key R&D Program of China(2016YFA0202900);the Key Program supportedby theNaturalScience Foundationof ZhejiangProvince,China(LZ18B060002);the Key R&D Project of Zhejiang Province(2020C01133).

摘　　要：Selective hydrogenation of phenol to cyclohexanone is intriguing in chemical industry.Though a few catalysts with promising performances have been developed in recent years,the basic principle for catalyst design is still missing owing to the unclear catalytic mechanism.This work tries to unravel the mechanism of phenol hydro-genation and the reasons causing the selectivity discrepancy on noble metal catalysts under mild conditions.Results show that different reaction pathways always firstly converge to the formation of cyclohexanone under mild conditions.The selectivity discrepancy mainly depends on the activity for cyclohexanone sequential hy-drogenation,in which two factors are found to be responsible,i.e.the hydrogenation energy barrier and the competitive chemisorption between phenol and cyclohexanone,if the specific co-catalyzing effect of H 2 O on Ru is not considered.Based on the above results,a quantitative descriptor,E b(one/pl)/E a,in which E a can be further correlated to the d band center of the noble metal catalyst,is proposed by the first time to roughly evaluate and predict the selectivity to cyclohexanone for catalyst screening.

关 键 词：PHENOL Selective hydrogenation CYCLOHEXANONE DFT Noble metal catalysts 

分 类 号：O624.421[理学—有机化学] O643.36[理学—化学]