Tuning CO2 hydrogenation selectivity via metal-oxide interfacial sites
Abstract
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 metal-oxide 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-FeOx 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-FeOx interfaces) promotes *CO desorption to increase CO selectivity, while moderate interaction (e.g., Ni-ZrO2 interfaces) facilitates further hydrogenation of *CO to produce CH4.
- Authors:
-
[4];
[5]
- Tsinghua Univ., Beijing (China); Brookhaven National Lab. (BNL), Upton, NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States); Tsinghua Univ., Beijing (China)
- Florida A&M Univ., Tallahassee, FL (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States);; Columbia Univ., New York, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1569545
- Alternate Identifier(s):
- OSTI ID: 1542480
- Report Number(s):
- BNL-212163-2019-JAAM
Journal ID: ISSN 0021-9517
- Grant/Contract Number:
- SC0012704; AC02-06CH11357; AC02-76SF00515; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Catalysis
- Additional Journal Information:
- Journal Volume: 374; Journal Issue: C; Journal ID: ISSN 0021-9517
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; Heterogeneous catalysis; CO2 hydrogenation; Active site; Metal-oxide interface; Selectivity
Citation Formats
Yan, Binhang, Zhao, Baohuai, Kattel, Shyam, Wu, Qiyuan, Yao, Siyu, Su, Dong, and Chen, Jingguang G. Tuning CO2 hydrogenation selectivity via metal-oxide interfacial sites. United States: N. p., 2019.
Web. doi:10.1016/j.jcat.2019.04.036.
Yan, Binhang, Zhao, Baohuai, Kattel, Shyam, Wu, Qiyuan, Yao, Siyu, Su, Dong, & Chen, Jingguang G. Tuning CO2 hydrogenation selectivity via metal-oxide interfacial sites. United States. https://doi.org/10.1016/j.jcat.2019.04.036
Yan, Binhang, Zhao, Baohuai, Kattel, Shyam, Wu, Qiyuan, Yao, Siyu, Su, Dong, and Chen, Jingguang G. Mon .
"Tuning CO2 hydrogenation selectivity via metal-oxide interfacial sites". United States. https://doi.org/10.1016/j.jcat.2019.04.036. https://www.osti.gov/servlets/purl/1569545.
@article{osti_1569545,
title = {Tuning CO2 hydrogenation selectivity via metal-oxide interfacial sites},
author = {Yan, Binhang and Zhao, Baohuai and Kattel, Shyam and Wu, Qiyuan and Yao, Siyu and Su, Dong and Chen, Jingguang G.},
abstractNote = {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 metal-oxide 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-FeOx 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-FeOx interfaces) promotes *CO desorption to increase CO selectivity, while moderate interaction (e.g., Ni-ZrO2 interfaces) facilitates further hydrogenation of *CO to produce CH4.},
doi = {10.1016/j.jcat.2019.04.036},
journal = {Journal of Catalysis},
number = C,
volume = 374,
place = {United States},
year = {Mon May 06 00:00:00 EDT 2019},
month = {Mon May 06 00:00:00 EDT 2019}
}
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