文献类型：期刊文献

英文题名：A promising low pressure methanol synthesis route from CO2 hydrogenation over Pd@Zn core-shell catalysts

作者：Liao, Fenglin[1];Wu, Xin-Ping[2,3];Zheng, Jianwei[4];Li, Molly Meng-Jung[1];Kroner, Anna[5];Zeng, Ziyan[6];Hong, Xinlin[6];Yuan, Youzhu[4];Gong, Xue-Qing[2,3];Tsang, Shik Chi Edman[1]

机构：[1]Univ Oxford, Dept Chem, Wolfson Catalysis Ctr, Oxford OX1 3QR, England;[2]East China Univ Sci & Technol, Coll Chem & Mol Engn, Ctr Computat Chem, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Coll Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[4]Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces,iChEM, Natl Engn Lab Green Chem Prod Alcohols Ethers Est, Xiamen 361005, Peoples R China;[5]Diamond Light Source Ltd, Harwell Sci & Innovat, Didcot OX11 0DE, Oxon, England;[6]Wuhan Univ, Dept Chem, Wuhan 430072, Peoples R China

年份：2017

卷号：19

期号：1

起止页码：270

外文期刊名：GREEN CHEMISTRY

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000391728900029)】；

基金：The authors wish to thank EPSRC, UK (Oxford) and NSFC-21421004, 21373153, 21322307, China for the financial support for this collaborative work and are grateful to the Chinese Scholarship Council (CSC) of China for granting a PhD scholarship to FL to work at Oxford. The ECUST group acknowledges the computing time at the National Super Computing Center in Jinan, China. The authors thank Diamond Light Source to allow a rapid access to the EXAFS facilities on B18.

语种：英文

摘要：At present, there is no low pressure methanol synthesis from CO2/H-2 with high yield despite the presence of an upstream process of aqueous phase reforming (APR) of biomass derivatives on an industrial scale for CO2/H-2 production at ca. 2 MPa. This is due to the intrinsic thermodynamics of the system which leads to particularly high CO levels at low pressure through reversed water gas shift reaction (RWGS) for most studied catalysts. Here we report a new Pd@Zn core-shell catalyst that offers a significantly higher kinetic barrier to CO/H2O formation in CO2 hydrogenation to reduce the CO levels but facilitates CH3OH formation at or below 2 MPa with CH3OH selectivity maintained at ca. 70% compared to ca. 10% over industrial Cu catalysts. The corresponding methanol yield at 2 MPa reaches 6.1 gmethanol gactive metal(-1) h(-1), which is comparable to the best reported value among a wide variety of catalysts under 5 MPa. It is thus believed that this active Pd based catalyst opens up a promising possibility for low pressure and temperature methanol production using a renewable biomass resource for fossil-fuel-starved countries.