Probing the surface chemistry for reverse water gas shift reaction on Pt(1 1 1) using ambient pressure X-ray photoelectron spectroscopy
Abstract
Using ambient pressure XPS (APXPS), we explored carbon dioxide (CO2) adsorption and CO2 hydrogenation on Pt(1 1 1) single crystal surface to observe the activation of CO2 and the subsequent reaction mechanism. In pure CO2, we observed CO adsorbates and adsorbed oxygen on Pt(1 1 1) derived from CO2 dissociation at room temperature. The introduction of H2 (at a pressure ratio of 1:1 (H2:CO2)) increased the production of CO across all temperatures by facilitating the removal of surface oxygen. As a consequence, the surface could expose sites that could then be utilized for producing CO. Under these conditions, the reverse water–gas shift (RWGS) reaction was observed starting at 300 °C. At higher H2 partial pressure (10:1 (H2:CO2)), the RWGS reaction initiated at a lower temperature of 200 °C and continued to enhance the conversion of CO2 with increasing temperatures. Our results revealed that CO2 was activated on a clean Pt(1 1 1) surface through the dissociation mechanism to form adsorbed CO and O at room temperature and at elevated temperatures. Introducing H2 facilitated the RWGS as adsorbed oxygen was consumed continuously to form H2O, and adsorbed CO desorbed from the surface at elevated temperatures. This work clearly provides direct experimentalmore »
- Authors:
-
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of Science and Technology of China, Hefei (China)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Gwangju Inst. of Science and Technology (Korea, Republic of)
- Univ. of Science and Technology of China, Hefei (China)
- Gwangju Inst. of Science and Technology (Korea, Republic of)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of Science and Technology of China, Hefei (China)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); China Scholarship Council (CSC)
- OSTI Identifier:
- 1841566
- Alternate Identifier(s):
- OSTI ID: 1761540; OSTI ID: 1841714
- Grant/Contract Number:
- AC02-05CH11231; 201706340112
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Catalysis
- Additional Journal Information:
- Journal Volume: 391; Journal ID: ISSN 0021-9517
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ambient pressure x-ray photoelectron; spectroscopy; surface catalysis; reverse water gas shift reaction; RWGS; APXPS; CO2 hydrogenation
Citation Formats
Su, Hongyang, Ye, Yifan, Lee, Kyung-Jae, Zeng, Jie, Mun, Bongjin S., and Crumlin, Ethan J. Probing the surface chemistry for reverse water gas shift reaction on Pt(1 1 1) using ambient pressure X-ray photoelectron spectroscopy. United States: N. p., 2020.
Web. doi:10.1016/j.jcat.2020.08.017.
Su, Hongyang, Ye, Yifan, Lee, Kyung-Jae, Zeng, Jie, Mun, Bongjin S., & Crumlin, Ethan J. Probing the surface chemistry for reverse water gas shift reaction on Pt(1 1 1) using ambient pressure X-ray photoelectron spectroscopy. United States. https://doi.org/10.1016/j.jcat.2020.08.017
Su, Hongyang, Ye, Yifan, Lee, Kyung-Jae, Zeng, Jie, Mun, Bongjin S., and Crumlin, Ethan J. Wed .
"Probing the surface chemistry for reverse water gas shift reaction on Pt(1 1 1) using ambient pressure X-ray photoelectron spectroscopy". United States. https://doi.org/10.1016/j.jcat.2020.08.017. https://www.osti.gov/servlets/purl/1841566.
@article{osti_1841566,
title = {Probing the surface chemistry for reverse water gas shift reaction on Pt(1 1 1) using ambient pressure X-ray photoelectron spectroscopy},
author = {Su, Hongyang and Ye, Yifan and Lee, Kyung-Jae and Zeng, Jie and Mun, Bongjin S. and Crumlin, Ethan J.},
abstractNote = {Using ambient pressure XPS (APXPS), we explored carbon dioxide (CO2) adsorption and CO2 hydrogenation on Pt(1 1 1) single crystal surface to observe the activation of CO2 and the subsequent reaction mechanism. In pure CO2, we observed CO adsorbates and adsorbed oxygen on Pt(1 1 1) derived from CO2 dissociation at room temperature. The introduction of H2 (at a pressure ratio of 1:1 (H2:CO2)) increased the production of CO across all temperatures by facilitating the removal of surface oxygen. As a consequence, the surface could expose sites that could then be utilized for producing CO. Under these conditions, the reverse water–gas shift (RWGS) reaction was observed starting at 300 °C. At higher H2 partial pressure (10:1 (H2:CO2)), the RWGS reaction initiated at a lower temperature of 200 °C and continued to enhance the conversion of CO2 with increasing temperatures. Our results revealed that CO2 was activated on a clean Pt(1 1 1) surface through the dissociation mechanism to form adsorbed CO and O at room temperature and at elevated temperatures. Introducing H2 facilitated the RWGS as adsorbed oxygen was consumed continuously to form H2O, and adsorbed CO desorbed from the surface at elevated temperatures. This work clearly provides direct experimental evidence for the surface chemistry of CO2 dissociation and demonstrates how hydrogen impacts the RWGS reaction on a platinum surface.},
doi = {10.1016/j.jcat.2020.08.017},
journal = {Journal of Catalysis},
number = ,
volume = 391,
place = {United States},
year = {Wed Aug 19 00:00:00 EDT 2020},
month = {Wed Aug 19 00:00:00 EDT 2020}
}
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