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Title: Complex catalytic behaviors of CuTiO x mixed-oxide during CO oxidation

Mixed metal oxides have attracted considerable attention in heterogeneous catalysis due to the unique stability, reactivity, and selectivity. Here, the activity and stability of the CuTiO x monolayer film supported on Cu(111), CuTiO x/Cu(111), during CO oxidation was explored using density functional theory (DFT). The unique structural frame of CuTiO x is able to stabilize and isolate a single Cu + site on the terrace, which is previously proposed active for CO oxidation. Furthermore, it is not the case, where the reaction via both the Langmuir–Hinshelwood (LH) and the Mars-van Krevelen (M-vK) mechanisms are hindered on such single Cu + site. Upon the formation of step-edges, the synergy among Cu δ+ sites, TiO x matrix, and Cu(111) is able to catalyze the reaction well. Depending on temperatures and partial pressure of CO and O 2, the surface structure varies, which determines the dominant mechanism. In accordance with our results, the Cu δ+ ion alone does not work well for CO oxidation in the form of single sites, while the synergy among multiple active sites is necessary to facilitate the reaction.
Authors:
 [1] ;  [2]
  1. Chungnam National Univ., Daejeon (Korea); Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Report Number(s):
BNL-108461-2015-JA
Journal ID: ISSN 1932-7447; R&D Project: 16068; KC0403020
Grant/Contract Number:
SC00112704
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 119; Journal Issue: 40; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
30 DIRECT ENERGY CONVERSION; CO oxidation; CuTiOx; mechanism; mixed oxide; DFT
OSTI Identifier:
1224192

Kim, Hyun You, and Liu, Ping. Complex catalytic behaviors of CuTiOx mixed-oxide during CO oxidation. United States: N. p., Web. doi:10.1021/acs.jpcc.5b07099.
Kim, Hyun You, & Liu, Ping. Complex catalytic behaviors of CuTiOx mixed-oxide during CO oxidation. United States. doi:10.1021/acs.jpcc.5b07099.
Kim, Hyun You, and Liu, Ping. 2015. "Complex catalytic behaviors of CuTiOx mixed-oxide during CO oxidation". United States. doi:10.1021/acs.jpcc.5b07099. https://www.osti.gov/servlets/purl/1224192.
@article{osti_1224192,
title = {Complex catalytic behaviors of CuTiOx mixed-oxide during CO oxidation},
author = {Kim, Hyun You and Liu, Ping},
abstractNote = {Mixed metal oxides have attracted considerable attention in heterogeneous catalysis due to the unique stability, reactivity, and selectivity. Here, the activity and stability of the CuTiOx monolayer film supported on Cu(111), CuTiOx/Cu(111), during CO oxidation was explored using density functional theory (DFT). The unique structural frame of CuTiOx is able to stabilize and isolate a single Cu+ site on the terrace, which is previously proposed active for CO oxidation. Furthermore, it is not the case, where the reaction via both the Langmuir–Hinshelwood (LH) and the Mars-van Krevelen (M-vK) mechanisms are hindered on such single Cu+ site. Upon the formation of step-edges, the synergy among Cuδ+ sites, TiOx matrix, and Cu(111) is able to catalyze the reaction well. Depending on temperatures and partial pressure of CO and O2, the surface structure varies, which determines the dominant mechanism. In accordance with our results, the Cuδ+ ion alone does not work well for CO oxidation in the form of single sites, while the synergy among multiple active sites is necessary to facilitate the reaction.},
doi = {10.1021/acs.jpcc.5b07099},
journal = {Journal of Physical Chemistry. C},
number = 40,
volume = 119,
place = {United States},
year = {2015},
month = {9}
}