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Title: Wet Chemical Growth and Thermocatalytic Activity of Cu-Based Nanoparticles Supported on TiO 2 Nanoparticles/HOPG: In Situ Ambient Pressure XPS Study of the CO 2 Hydrogenation Reaction

Abstract

The present study examines the synthesis of unique Cu nanostructured model catalysts and their catalytic activity toward CO 2 hydrogenation under moderate temperature and pressure reaction conditions. Cu-based nanoparticles (NPs) were synthesized by two chemical deposition methods: (1) 5 nm spherical Cu(OH) 2 NPs deposited on highly oriented pyrolytic graphite (HOPG) by exposing the HOPG substrate to a colloidal solution of copper, and (2) photocatalytic reduction of [Cu(H 2O) 6] 2+ onto a high density of 15 nm TiO 2 NPs grown on HOPG by physical vapor deposition. This photocatalytic reduction results in the deposition of mixed Cu(OH) 2 and Cu 2O films, while few-nm sized Cu-based NPs are formed on the TiO 2 NPs upon subsequent reduction. The chemistry, structure, and morphology of the resulting samples were characterized using X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and scanning electron microscopy (SEM). The thermocatalytic activity for the CO 2 reduction reaction (CO 2RR) under H 2 was evaluated with synchrotron-based ambient pressure X-ray photoelectron spectroscopy (AP-XPS) and temperature-programmed desorption (TPD) experiments. Several intermediates, including CO 2 δ–, HCOO, O–CH 3, CO 3 2–, CH x, and CO, were observed using AP-XPS. The TiO 2 NPs show activity toward themore » formation of methanol (CH3OH) that occurs mainly through an O–CH 3 intermediate. The TiO 2 NPs-core–carbon-shell (TiO 2@C NPs) shows a clear selectivity toward methane (CH 4).« less

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of California, Irvine, CA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
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:
1569558
Report Number(s):
BNL-212139-2019-JAAM
Journal ID: ISSN 2155-5435
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 9; Journal Issue: 8; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Ferrah, Djawhar, Haines, Amanda R., Galhenage, Randima P., Bruce, Jared P., Babore, Anthony D., Hunt, Adrian, Waluyo, Iradwikanari, and Hemminger, John C. Wet Chemical Growth and Thermocatalytic Activity of Cu-Based Nanoparticles Supported on TiO2 Nanoparticles/HOPG: In Situ Ambient Pressure XPS Study of the CO2 Hydrogenation Reaction. United States: N. p., 2019. Web. doi:10.1021/acscatal.9b01419.
Ferrah, Djawhar, Haines, Amanda R., Galhenage, Randima P., Bruce, Jared P., Babore, Anthony D., Hunt, Adrian, Waluyo, Iradwikanari, & Hemminger, John C. Wet Chemical Growth and Thermocatalytic Activity of Cu-Based Nanoparticles Supported on TiO2 Nanoparticles/HOPG: In Situ Ambient Pressure XPS Study of the CO2 Hydrogenation Reaction. United States. doi:10.1021/acscatal.9b01419.
Ferrah, Djawhar, Haines, Amanda R., Galhenage, Randima P., Bruce, Jared P., Babore, Anthony D., Hunt, Adrian, Waluyo, Iradwikanari, and Hemminger, John C. Tue . "Wet Chemical Growth and Thermocatalytic Activity of Cu-Based Nanoparticles Supported on TiO2 Nanoparticles/HOPG: In Situ Ambient Pressure XPS Study of the CO2 Hydrogenation Reaction". United States. doi:10.1021/acscatal.9b01419. https://www.osti.gov/servlets/purl/1569558.
@article{osti_1569558,
title = {Wet Chemical Growth and Thermocatalytic Activity of Cu-Based Nanoparticles Supported on TiO2 Nanoparticles/HOPG: In Situ Ambient Pressure XPS Study of the CO2 Hydrogenation Reaction},
author = {Ferrah, Djawhar and Haines, Amanda R. and Galhenage, Randima P. and Bruce, Jared P. and Babore, Anthony D. and Hunt, Adrian and Waluyo, Iradwikanari and Hemminger, John C.},
abstractNote = {The present study examines the synthesis of unique Cu nanostructured model catalysts and their catalytic activity toward CO2 hydrogenation under moderate temperature and pressure reaction conditions. Cu-based nanoparticles (NPs) were synthesized by two chemical deposition methods: (1) 5 nm spherical Cu(OH)2 NPs deposited on highly oriented pyrolytic graphite (HOPG) by exposing the HOPG substrate to a colloidal solution of copper, and (2) photocatalytic reduction of [Cu(H2O)6]2+ onto a high density of 15 nm TiO2 NPs grown on HOPG by physical vapor deposition. This photocatalytic reduction results in the deposition of mixed Cu(OH)2 and Cu2O films, while few-nm sized Cu-based NPs are formed on the TiO2 NPs upon subsequent reduction. The chemistry, structure, and morphology of the resulting samples were characterized using X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and scanning electron microscopy (SEM). The thermocatalytic activity for the CO2 reduction reaction (CO2RR) under H2 was evaluated with synchrotron-based ambient pressure X-ray photoelectron spectroscopy (AP-XPS) and temperature-programmed desorption (TPD) experiments. Several intermediates, including CO2δ–, HCOO, O–CH3, CO32–, CHx, and CO, were observed using AP-XPS. The TiO2 NPs show activity toward the formation of methanol (CH3OH) that occurs mainly through an O–CH3 intermediate. The TiO2 NPs-core–carbon-shell (TiO2@C NPs) shows a clear selectivity toward methane (CH4).},
doi = {10.1021/acscatal.9b01419},
journal = {ACS Catalysis},
issn = {2155-5435},
number = 8,
volume = 9,
place = {United States},
year = {2019},
month = {6}
}

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