文献类型：期刊文献

英文题名：Comparison of two multifunctional catalysts [M/Nb2O5 (M = Pd, Pt)] for one-pot hydrodeoxygenation of lignin

作者：Dong, Lin[1];Shao, Yi[1];Han, Xue[2];Liu, Xiaohui[1];Xia, Qineng[3];Parker, Stewart F.[4];Cheng, Yongqiang[5];Daemen, Luke L.[5];Ramirez-Cuesta, Anibal J.[5];Wang, Yanqin[1];Yang, Sihai[2]

机构：[1]East China Univ Sci & Technol, Shanghai Key Lab Funct Mat Chem, Res Inst Ind Catalysis, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[2]Univ Manchester, Sch Chem, Manchester M13 9PL, Lancs, England;[3]Jiaxing Univ, Sch Biol & Chem Engn, Jiaxing 314001, Zhejiang, Peoples R China;[4]STFC Rutherford Appleton Lab, ISIS Facil, Chilton OX11 0QX, Oxon, England;[5]Oak Ridge Natl Lab, CEMD, Neutron Sci Directorate, Oak Ridge, TN 37831 USA

年份：2018

卷号：8

期号：23

起止页码：6129

外文期刊名：CATALYSIS SCIENCE & TECHNOLOGY

收录：;EI(收录号：20184906176367);WOS:【SCI-EXPANDED(收录号:WOS:000451533800012)】；

基金：We thank the National Natural Science Foundation of China (No. 91545103, 21603072, 21832002, 21872050, 21808063), the Fundamental Research Funds for the Central Universities (222201718003, 222201817022), the Science and Technology Commission of Shanghai Municipality (10dz2220500), EPSRC (EP/P011632/1) and the University of Manchester for funding. We especially thank ORNL/SNS and STFC/ISIS for the access to the neutron scattering beamlines VISION and TOSCA, respectively. We are also grateful to ORNL and STFC for the computing resources.

语种：英文

外文关键词：Neutron scattering - Catalyst selectivity - Catalyst activity - Hydrogenation - Palladium compounds - Reaction kinetics

摘要：Improved lignin valorisation via its catalytic conversion to value-added feedstocks is of essential importance to the development of future bio-refineries. The identification of active binding domains within a catalyst structure provides important insights into the function of catalysts. Vibrational analysis employing inelastic neutron scattering (INS) enables the full investigation of the dynamics of hydrogen in host-guest systems. Here, we report an in situ INS investigation of the catalytic origins of two multifunctional catalysts [M/Nb2O5 (M = Pd, Pt)] for the hydrodeoxygenation (HDO) of phenol, a key model compound for lignin. We also report the excellent activity of these two catalysts for the conversion of raw lignin into hydrocarbons showing (i) complete removal of the oxygen content; (ii) near-quantitative yields of C-7-C-9 products based upon lignin monomers and (iii) different reaction networks. The in situ INS study has revealed the molecular details directly underpinning the distinct reaction pathways. We found that on the Pd/Nb2O5 catalyst, the hydrogenation of phenyl rings has higher selectivity than the direct cleavage of C-O bonds owing to the strong binding of the phenyl ring to the catalyst surface and the high hydrogenation activity of Pd, while on the Pt/Nb2O5 catalyst, the HDO reaction undergoes a combination of a direct dehydroxylation (DDO) process and a tandem route with fast kinetics, leading to a higher selectivity for arenes than that over Pd/Nb2O5 at the beginning of the reaction.