Understanding the promotional effects of trace doped Zn in Co/NC for efficient one-pot catalytic conversion of furfural to 2-methyl-tetrahydrofuran  

作　　者：Lei Huang Liqiang Wang Zonghao Zhang Xinpeng Guo Xiaowen Zhang Johnny Muya Chabu Pingle Liu Feiying Tang 

机构地区：[1]College of Chemical Engineering,Xiangtan University,Xiangtan 411105,Hunan,China [2]Henan Province Industrial Technology Research Institute of Resources and Materials,School of Material Science and Engineering,Zhengzhou University,Zhengzhou 450001,Henan,China [3]Department of Chemistry,Faculty of Science,University of Lubumbashi,PO Box 1825,Lubumbashi,DR,Congo [4]Foshan Green Intelligent Manufacturing Research Institute of Xiangtan University,Foshan 528010,Guangdong,China

出　　处：《Journal of Energy Chemistry》2022年第8期225-233,I0007,共10页能源化学（英文版）

基　　金：supported by the National Natural Science Foundation of China(22078277 and 21908185);the Project of Hunan Provincial Natural Science Foundation of China(2020JJ5532 and 2021JJ30658);the Degree&Postgraduate Education Reform Project of Hunan Provincial(XDCX2019B095 and CX20190489);the Guang Dong Basic and Applied Basic Research Foundation(2021A1515110789 and 2021A1515110136);the Science and Technology Innovation Program of Hunan Province(2021RC2089);the Research Initiation Project of Xiangtan University(KZ08076);the Environment-friendly Chemical Process Integration Technology Hunan Province Key Laboratory;the Collaborative Innovation Center of New Chemical Technologies for Environmental Benignity and Efficient Resource Utilization。

摘　　要：2-methyl-tetrahydrofuran(2-MTHF)is a promising biofuel or fuel additive with excellent burning property,a versatile new-style solvent in organic synthesis,and an important medical intermediate.In this work,a one-pot selective conversion of furfural(FA)into 2-MTHF was carried out over Zn doped Co/NC catalysts.The Zn-Co/NC-1 catalyst with trace Zn dopant(0.38 wt%)exhibited the best performance(yield of 2-MTHF:93.8%).According to the characterizations,it was found that the Zn not only incorporates into the carbon support but also partially dopes into Co nanoparticles.Subsequently,theoretical calculations demonstrated that the doping of Zn in carbon support can effectively enhance the electron transfer from the support to the metallic Co particle,leading to the electron-rich Co surface.The presence of Zn was found to promote the dissociation of hydrogen and to lower the diffusion barrier of hydrogen atom,in favor of the hydrogenation/hydrodeoxygenation processes.Furthermore,the Zn doped models exhibit much lower barrier in breaking C–OH bond of FOL,resulting in higher activity for hydrodeoxygenation of FOL.These theoretical results are consistent with the in situ FT-IR analysis of adsorption substrates and intermediates over Zn doped catalyst.This work reveals the mechanism of dopant Zn tailoring the electronic structure and catalytic performance of active sites,providing a deep insight into the design of economical and high-performance catalysts for hydrogenation/hydrodeoxygenation of biomass feedstocks.

关 键 词：Zn-doping Enhanced electron transfer Biomass upgrade FURFURAL 2-Methyl-tetrahydrofuran 

分 类 号：TQ251.1[化学工程—有机化工] O643.36[理学—物理化学]