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Title: Soft X-ray spectroscopy studies of adsorption and reaction of CO in the presence of H2 over 6 nm MnO nanoparticles supported on mesoporous Co3O4

Abstract

MnO nanoparticles (6 nm) were supported on mesoporous spinel Co3O4 and studied using ambient pressure X-ray photoelectron spectroscopy (APXPS) and in situ X-ray absorption spectroscopy (XAS) during hydrogenation of CO. The nature and evolution of surface adsorbed species as well as the oxidation states of the metal oxide surfaces were evaluated under oxidizing, reducing, and H2 + CO (2:1) reaction atmospheres. From APXPS, MnO nanoparticle surfaces were found to be progressively reduced in H2 atmospheres with increasing temperature. Surface adsorbed CO was found to be formed at the expense of lattice O under H2 + CO reaction conditions. In situ XAS indicated that the dominant oxide species were Co(OH)2, Co (II) oxides, MnO, and Mn3O4 under reaction conditions. In situ XAS also indicated the formation of gas phase CO2, the disappearance of lattice O, and the further reduction of Mn3O4 to MnO upon prolonged reaction in H2 + CO. Mass spectroscopy measurements showed the formation of CO2 and hydrocarbons. Finally, the spent catalyst was investigated using scanning transmission X-ray microscopy and (scanning) transmission electron microscopy; the catalyst grains were found to be homogeneous.

Authors:
 [1];  [1];  [1];  [1];  [1];  [2];  [3];  [2];  [1]; ORCiD logo [2]
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  1. University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  2. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1532189
Alternate Identifier(s):
OSTI ID: 1251759
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Surface Science
Additional Journal Information:
Journal Volume: 648; Journal Issue: C; Journal ID: ISSN 0039-6028
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ambient pressure x-ray photoelectron spectroscopy; in situ x-ray absorption spectroscopy; manganese oxide nanoparticles; mesoporous spinel cobalt oxide; CO hydrogenation

Citation Formats

Ralston, Walter T., Musselwhite, Nathan, Kennedy, Griffin, An, Kwangjin, Horowitz, Yonatan, Cordones, Amy A., Rude, Bruce, Ahmed, Musahid, Melaet, Gerome, and Alayoglu, Selim. Soft X-ray spectroscopy studies of adsorption and reaction of CO in the presence of H2 over 6 nm MnO nanoparticles supported on mesoporous Co3O4. United States: N. p., 2015. Web. doi:10.1016/j.susc.2015.12.006.
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Ralston, Walter T., Musselwhite, Nathan, Kennedy, Griffin, An, Kwangjin, Horowitz, Yonatan, Cordones, Amy A., Rude, Bruce, Ahmed, Musahid, Melaet, Gerome, & Alayoglu, Selim. Soft X-ray spectroscopy studies of adsorption and reaction of CO in the presence of H2 over 6 nm MnO nanoparticles supported on mesoporous Co3O4. United States. https://doi.org/10.1016/j.susc.2015.12.006
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Ralston, Walter T., Musselwhite, Nathan, Kennedy, Griffin, An, Kwangjin, Horowitz, Yonatan, Cordones, Amy A., Rude, Bruce, Ahmed, Musahid, Melaet, Gerome, and Alayoglu, Selim. Wed . "Soft X-ray spectroscopy studies of adsorption and reaction of CO in the presence of H2 over 6 nm MnO nanoparticles supported on mesoporous Co3O4". United States. https://doi.org/10.1016/j.susc.2015.12.006. https://www.osti.gov/servlets/purl/1532189.
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@article{osti_1532189,
title = {Soft X-ray spectroscopy studies of adsorption and reaction of CO in the presence of H2 over 6 nm MnO nanoparticles supported on mesoporous Co3O4},
author = {Ralston, Walter T. and Musselwhite, Nathan and Kennedy, Griffin and An, Kwangjin and Horowitz, Yonatan and Cordones, Amy A. and Rude, Bruce and Ahmed, Musahid and Melaet, Gerome and Alayoglu, Selim},
abstractNote = {MnO nanoparticles (6 nm) were supported on mesoporous spinel Co3O4 and studied using ambient pressure X-ray photoelectron spectroscopy (APXPS) and in situ X-ray absorption spectroscopy (XAS) during hydrogenation of CO. The nature and evolution of surface adsorbed species as well as the oxidation states of the metal oxide surfaces were evaluated under oxidizing, reducing, and H2 + CO (2:1) reaction atmospheres. From APXPS, MnO nanoparticle surfaces were found to be progressively reduced in H2 atmospheres with increasing temperature. Surface adsorbed CO was found to be formed at the expense of lattice O under H2 + CO reaction conditions. In situ XAS indicated that the dominant oxide species were Co(OH)2, Co (II) oxides, MnO, and Mn3O4 under reaction conditions. In situ XAS also indicated the formation of gas phase CO2, the disappearance of lattice O, and the further reduction of Mn3O4 to MnO upon prolonged reaction in H2 + CO. Mass spectroscopy measurements showed the formation of CO2 and hydrocarbons. Finally, the spent catalyst was investigated using scanning transmission X-ray microscopy and (scanning) transmission electron microscopy; the catalyst grains were found to be homogeneous.},
doi = {10.1016/j.susc.2015.12.006},
journal = {Surface Science},
number = C,
volume = 648,
place = {United States},
year = {Wed Dec 23 00:00:00 EST 2015},
month = {Wed Dec 23 00:00:00 EST 2015}
}
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https://doi.org/10.1016/j.susc.2015.12.006
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