Tuning CO2 hydrogenation selectivity via metal-oxide interfacial sites

被引:124
|
作者
Yan, Binhang [1 ,2 ]
Zhao, Baohuai [2 ,3 ]
Kattel, Shyam [4 ]
Wu, Qiyuan [5 ]
Yao, Siyu [2 ]
Su, Dong [5 ]
Chen, Jingguang G. [2 ,6 ]
机构
[1] Tsinghua Univ, Dept Chem Engn, Beijing 100084, Peoples R China
[2] Brookhaven Natl Lab, Chem Dept, Upton, NY 11973 USA
[3] Tsinghua Univ, Coll Mat Sci & Engn, Beijing 100084, Peoples R China
[4] Florida A&M Univ, Dept Phys, Tallahassee, FL 32307 USA
[5] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA
[6] Columbia Univ, Dept Chem Engn, New York, NY 10027 USA
关键词
Heterogeneous catalysis; CO2; hydrogenation; Active site; Metal-oxide interface; Selectivity; DENSITY-FUNCTIONAL THEORY; TOTAL-ENERGY CALCULATIONS; CARBON-DIOXIDE; BIMETALLIC CATALYSTS; METHANATION REACTION; METHANOL SYNTHESIS; SURFACE; REDUCTION; MECHANISMS; ADSORPTION;
D O I
10.1016/j.jcat.2019.04.036
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
CO2 hydrogenation over ZrO2-supported NiFe catalysts is investigated to illustrate the role of Fe in controlling the activity and selectivity, and to reveal the structure-function relationship between metaloxide interfaces and catalytic selectivities. The Ni-ZrO2 interfaces and Ni-FeOx interfaces are identified as the most likely active sites for the methanation reaction and the reverse water-gas shift reaction, respectively, using combined in-situ and ex-situ characterization techniques. The reaction mechanisms of CO2 hydrogenation to CH4 on the Ni-ZrO2 interfacial sites and to CO on the Ni-FeO C interfacial sites are further revealed by combined in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations. Both experimental and theoretical results demonstrate that the binding energy of absorbed CO (*CO) is a key descriptor to predict CO2 hydrogenation selectivity: weak interaction (e.g., Ni-Fe0 x interfaces) promotes *CO desorption to increase CO selectivity, while moderate interaction (e.g., Ni-ZrO2 interfaces) facilitates further hydrogenation of *CO to produce CH4. (C) 2019 Elsevier Inc. All rights reserved.
引用
收藏
页码:60 / 71
页数:12
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