Growth, Structure, and Catalytic Properties of ZnOx Grown on CuOx/Cu(111) Surfaces
Abstract
A catalyst with a ZnO/Cu configuration plays an important role in the synthesis of methanol from CO2 hydrogenation. In this study, scanning tunneling microscopy and X-ray photoelectron spectroscopy (XPS) were used to investigate the growth mode of small coverages of ZnOx, θoxi < 0.3 monolayer, on a Cu(111) substrate. Our results show that the modes of growth, size, and shape of the ZnO nanoparticles are strongly dependent on the Zn deposition temperature. In a set of experiments, Zn was deposited on Cu(111) or CuOx/Cu(111) surfaces at 300 K with subsequent exposure to O2 at higher temperatures (400–550 K), which exhibited small particles of ZnO (<20 nm in size) on the surface. The deposition of Zn onto CuOx/Cu(111) at elevated temperatures (450–600 K) in an oxygen ambient produced large ZnO islands (300–650 nm in size), which were very rough and spread over several terraces of Cu(111). XPS/Auger spectra showed that all of the preparation conditions stated above led to the formation ZnO/CuOx/Cu(111) surfaces where the oxidation state of zinc was uniform. In conclusion, catalytic tests showed that all these surfaces were active for the hydrogenation of CO2 to methanol, but only the systems prepared at 600 K displayed long-term stability undermore »
- Authors:
-
- Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.
- State Univ. of New York (SUNY) at Stony Brook, Stony Brook, NY (United States). Dept. of Chemistry
- Univ. Central de Venezuela, Caracas (Venezuela). Facultad de Ciencias
- Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.; Univ. Central de Venezuela, Caracas (Venezuela). Facultad de Ciencias
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1484882
- Report Number(s):
- BNL-209648-2018-JAAM
Journal ID: ISSN 1932-7447
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 122; Journal Issue: 46; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
Citation Formats
Mahapatra, Mausumi, Kang, Jindong, Ramírez, Pedro J., Hamlyn, Rebecca, Rui, Ning, Liu, Zongyuan, Orozco, Ivan, Senanayake, Sanjaya D., and Rodriguez, José A. Growth, Structure, and Catalytic Properties of ZnOx Grown on CuOx/Cu(111) Surfaces. United States: N. p., 2018.
Web. doi:10.1021/acs.jpcc.8b09243.
Mahapatra, Mausumi, Kang, Jindong, Ramírez, Pedro J., Hamlyn, Rebecca, Rui, Ning, Liu, Zongyuan, Orozco, Ivan, Senanayake, Sanjaya D., & Rodriguez, José A. Growth, Structure, and Catalytic Properties of ZnOx Grown on CuOx/Cu(111) Surfaces. United States. https://doi.org/10.1021/acs.jpcc.8b09243
Mahapatra, Mausumi, Kang, Jindong, Ramírez, Pedro J., Hamlyn, Rebecca, Rui, Ning, Liu, Zongyuan, Orozco, Ivan, Senanayake, Sanjaya D., and Rodriguez, José A. Tue .
"Growth, Structure, and Catalytic Properties of ZnOx Grown on CuOx/Cu(111) Surfaces". United States. https://doi.org/10.1021/acs.jpcc.8b09243. https://www.osti.gov/servlets/purl/1484882.
@article{osti_1484882,
title = {Growth, Structure, and Catalytic Properties of ZnOx Grown on CuOx/Cu(111) Surfaces},
author = {Mahapatra, Mausumi and Kang, Jindong and Ramírez, Pedro J. and Hamlyn, Rebecca and Rui, Ning and Liu, Zongyuan and Orozco, Ivan and Senanayake, Sanjaya D. and Rodriguez, José A.},
abstractNote = {A catalyst with a ZnO/Cu configuration plays an important role in the synthesis of methanol from CO2 hydrogenation. In this study, scanning tunneling microscopy and X-ray photoelectron spectroscopy (XPS) were used to investigate the growth mode of small coverages of ZnOx, θoxi < 0.3 monolayer, on a Cu(111) substrate. Our results show that the modes of growth, size, and shape of the ZnO nanoparticles are strongly dependent on the Zn deposition temperature. In a set of experiments, Zn was deposited on Cu(111) or CuOx/Cu(111) surfaces at 300 K with subsequent exposure to O2 at higher temperatures (400–550 K), which exhibited small particles of ZnO (<20 nm in size) on the surface. The deposition of Zn onto CuOx/Cu(111) at elevated temperatures (450–600 K) in an oxygen ambient produced large ZnO islands (300–650 nm in size), which were very rough and spread over several terraces of Cu(111). XPS/Auger spectra showed that all of the preparation conditions stated above led to the formation ZnO/CuOx/Cu(111) surfaces where the oxidation state of zinc was uniform. In conclusion, catalytic tests showed that all these surfaces were active for the hydrogenation of CO2 to methanol, but only the systems prepared at 600 K displayed long-term stability under reaction conditions.},
doi = {10.1021/acs.jpcc.8b09243},
journal = {Journal of Physical Chemistry. C},
number = 46,
volume = 122,
place = {United States},
year = {Tue Oct 30 00:00:00 EDT 2018},
month = {Tue Oct 30 00:00:00 EDT 2018}
}
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