文献类型：期刊文献

英文题名：Cooperative Catalysis of Nickel and Nickel Oxide for Efficient Reduction of CO2 to CH4

作者：Bi, Qingyuan[1];Huang, Xieyi[1];Yin, Guoheng[1];Chen, Tianyuan[2];Du, Xianlong[3];Cai, Jun[4,5];Xu, Jing[2];Liu, Zhi[4,5];Han, Yifan[2];Huang, Fuqiang[1,5,6]

机构：[1]Chinese Acad Sci, State Key Lab High Performance Ceram & Superfine, Shanghai Inst Ceram, Shanghai 200050, Peoples R China;[2]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[3]Chinese Acad Sci, Key Lab Interfacial Phys & Technol, Shanghai Inst Appl Phys, Shanghai 201800, Peoples R China;[4]Chinese Acad Sci, State Key Lab Funct Mat Informat, Shanghai Inst Microsyst & Informat Technol, Shanghai 200050, Peoples R China;[5]ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201203, Peoples R China;[6]Peking Univ, State Key Lab Rare Earth Mat Chem & Applicat, Coll Chem & Mol Engn, Beijing 100871, Peoples R China

年份：2019

卷号：11

期号：4

起止页码：1295

外文期刊名：CHEMCATCHEM

收录：;EI(收录号：20190506441834);WOS:【SCI-EXPANDED(收录号:WOS:000459333500021)】；

基金：This work was supported by the National Key Research and Development Program of China (2016YFB0901600), the NSF of China (21872166 and 51502331), the STC of Shanghai (16ZR1440400 and 16JC1401700), and the Key Research Program of Chinese Academy of Sciences (KGZD-EW-T06 and QYZDJ-SSW-JSC013).

语种：英文

外文关键词：CH4 generation; CO2 utilization; active sites; cooperative catalysis; Ni-NiO components

摘要：The use of CO2 to produce value-added energy chemicals is a promising means for renewable CO2 transformation in low-carbon energy system, and CO2 methanation has attracted ever-increasing interest. Herein, we report that the Ni/MCM-41 catalyst with prominent cooperative effect of Ni and NiO is efficient for CH4 generation with CO2 conversion of 73.2 % and CH4 selectivity of 91.6 % at 400 degrees C and high gas hourly space velocity (GHSV) of 90000 mL g(cat)(-1) h(-1). Combined methodologies of in situ X-ray diffraction, diffuse reflectance infrared Fourier transform spectroscopy, and ambient-pressure X-ray photoelectron spectroscopy reflect the structural evolvements of Ni/MCM-41 catalyst, the presence of carbonyl intermediates, the co-existence of metallic and oxidized Ni species with sufficient molar ratio of Ni-0/Ni2+ under working conditions. H-2 and CO2 molecules are preferentially adsorbed and chemically activated over Ni-0 and Ni2+ species, respectively. The possible four-step reaction mechanism involved carbonyl pathway and the cleavage of C=O bond from CO2 as the rate-determining step over the engineered Ni/MCM-41 catalyst was demonstrated.