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Title: Strongly Modified Scaling of CO Hydrogenation in Metal Supported TiO Nanostripes

Abstract

The boundary between a metal-oxide and its metal support (metal-oxide|support) provides an intriguing structural interface for heterogeneous catalysis. The hydrogenation of CO is a reaction step believed to be rate limiting in electro-chemical CO2 reduction. Density functional theory (DFT) calculations were performed to study this reaction step for a class of catalytic material: metal supported TiO nanostripe. The most stable adsorption sites were identified for all metal supports which showed a striking difference in adsorbate geometry between the strong and weak binding metal supports. The modified CO hydrogenation scaling shows a significant strengthening over (111) and (211) transition metal surfaces. Such enhancement can be attributed to a combination of geometrical effects and metal-oxide|support electronic interactions. A correlation analysis was performed to identify the key features needed to accurately predict *CO and *CHO adsorption energies on the TiO nanostripes and to further validate our physical analysis of the results. This structural motif seems to be a promising avenue to explore scaling modification in other metal-oxide materials and reactions.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [2]; ORCiD logo [2]
  1. Stanford Univ., Stanford, CA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  3. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States); Technical Univ. of Denmark, Lyngby (Denmark)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1490983
Alternate Identifier(s):
OSTI ID: 1490748
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 8; Journal Issue: 11; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO hydrogenation; CO2 reduction; computational catalysis; DFT; metal-oxides; nanostripe; scaling relations; ultrathin overlayers

Citation Formats

Sandberg, Robert B., Hansen, Martin H., Nørskov, Jens K., Abild-Pedersen, Frank, and Bajdich, Michal. Strongly Modified Scaling of CO Hydrogenation in Metal Supported TiO Nanostripes. United States: N. p., 2018. Web. https://doi.org/10.1021/acscatal.8b03327.
Sandberg, Robert B., Hansen, Martin H., Nørskov, Jens K., Abild-Pedersen, Frank, & Bajdich, Michal. Strongly Modified Scaling of CO Hydrogenation in Metal Supported TiO Nanostripes. United States. https://doi.org/10.1021/acscatal.8b03327
Sandberg, Robert B., Hansen, Martin H., Nørskov, Jens K., Abild-Pedersen, Frank, and Bajdich, Michal. Wed . "Strongly Modified Scaling of CO Hydrogenation in Metal Supported TiO Nanostripes". United States. https://doi.org/10.1021/acscatal.8b03327. https://www.osti.gov/servlets/purl/1490983.
@article{osti_1490983,
title = {Strongly Modified Scaling of CO Hydrogenation in Metal Supported TiO Nanostripes},
author = {Sandberg, Robert B. and Hansen, Martin H. and Nørskov, Jens K. and Abild-Pedersen, Frank and Bajdich, Michal},
abstractNote = {The boundary between a metal-oxide and its metal support (metal-oxide|support) provides an intriguing structural interface for heterogeneous catalysis. The hydrogenation of CO is a reaction step believed to be rate limiting in electro-chemical CO2 reduction. Density functional theory (DFT) calculations were performed to study this reaction step for a class of catalytic material: metal supported TiO nanostripe. The most stable adsorption sites were identified for all metal supports which showed a striking difference in adsorbate geometry between the strong and weak binding metal supports. The modified CO hydrogenation scaling shows a significant strengthening over (111) and (211) transition metal surfaces. Such enhancement can be attributed to a combination of geometrical effects and metal-oxide|support electronic interactions. A correlation analysis was performed to identify the key features needed to accurately predict *CO and *CHO adsorption energies on the TiO nanostripes and to further validate our physical analysis of the results. This structural motif seems to be a promising avenue to explore scaling modification in other metal-oxide materials and reactions.},
doi = {10.1021/acscatal.8b03327},
journal = {ACS Catalysis},
number = 11,
volume = 8,
place = {United States},
year = {2018},
month = {10}
}

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Cited by: 3 works
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Figures / Tables:

Figure 1 Figure 1: Energy of a free-standing TiO overlayer as a function of hexagonal lattice constant. Dashed lines show the corresponding metal-metal distances in ( ll l) surfaces offcc support metals used in this study. The two minima at 3.10 and 3.33 Å correspond to the original rocksalt and stretched TiOmore » geometries, shown as insets.« less

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