文献类型：期刊文献

英文题名：Vacancy engineering of the nickel-based catalysts for enhanced CO2 methanation

作者：Zhu, Minghui[1];Tian, Pengfei[1];Cao, Xinyu[1];Chen, Jiacheng[1];Pu, Tiancheng[1];Shi, Bianfang[1];Xu, Jing[1];Moon, Jisue[2,3];Wu, Zili[2,3];Han, Yi-Fan[1,4]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Sch Chem Engn, Shanghai 200237, Peoples R China;[2]Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA;[3]Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA;[4]Zhengzhou Univ, Engn Res Ctr Adv Funct Mat Mfg, Minist Educ, Zhengzhou 450001, Peoples R China

年份：2021

卷号：282

外文期刊名：APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY

收录：;EI(收录号：20203909249748);WOS:【SCI-EXPANDED(收录号:WOS:000591695500008)】；

基金：This work was sponsored by the National Key R&D Program of China (2018YFB0604501), the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, Shanghai Sailing Program (19YF1410600) and the Fundamental Research Funds for the Central Universities (JKA012016018). JM and ZW were supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science program.

语种：英文

外文关键词：CO(2)methanation; Oxygen defect; Nickel-based catalysts; Cerium oxide; Spectrokinetics

摘要：It is challenging to elucidate the mechanism of CO2 methanation reaction over nickel-based catalysts and precisely tune the kinetics of rate-determining-step. In this work, we propose a strategy to engineer the oxygen vacancies of nickel-based catalysts for enhanced CO2 methanation. A Y2O3-promoted NiO-CeO2 catalyst is prepared and found to exhibit an outstanding methanation activity that is up to three folds higher than NiO-CeO2 and six folds higher than NiO-Y2O3 at mild reaction temperatures (< 300 degrees C). We demonstrate both theoretically and experimentally that the introduction of Y2O3 to CeO2 greatly facilitates the generation of surface oxygen vacancies during the reaction. Using spectrokinetics analysis, we further revealed that these sites promote the direct dissociation of CO2, which is kinetically more favorable than the associative route. Thus, it dramatically improved the CO2 methanation activity. The vacancy engineering strategy will potentially guide the rational design of a broad range of heterogeneous catalysts for CO2 hydrogenation.