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Title: Structure-Sensitive Scaling Relations: Adsorption Energies from Surface Site Stability

Abstract

Here, the design of heterogeneous catalysts is accelerated by the identification of thermochemical reactivity descriptors, which enable the prediction of promising materials through efficient screening. Motivated by previous discoveries of linear scaling relations between the adsorption energies of related atoms and molecules, we present a new scaling between the adsorption energies of metal atoms and metal–adsorbate complexes, which can be used to directly predict catalytically relevant molecular adsorption energies. In contrast to existing models based on the coordination number of surface atoms alone, our model can predict adsorption energies with site–by–site resolution considering local structural effects and also has potential extensions to include contributions of neighboring metal identity in alloy systems. Integration of this scaling with a previously identified model for metal–metal interactions enables the accurate prediction of molecular adsorption energies on nanoparticles by performing only a small set of slab–based calculations.

Authors:
ORCiD logo [1];  [2]
  1. Stanford Univ., Stanford, CA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1457171
Alternate Identifier(s):
OSTI ID: 1423493
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ChemCatChem
Additional Journal Information:
Journal Volume: 10; Journal Issue: 7; Journal ID: ISSN 1867-3880
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; coordination number; density functional theory; heterogeneous catalysis; nanoparticles; transition metals

Citation Formats

Roling, Luke T., and Abild-Pedersen, Frank. Structure-Sensitive Scaling Relations: Adsorption Energies from Surface Site Stability. United States: N. p., 2017. Web. doi:10.1002/cctc.201701841.
Roling, Luke T., & Abild-Pedersen, Frank. Structure-Sensitive Scaling Relations: Adsorption Energies from Surface Site Stability. United States. doi:10.1002/cctc.201701841.
Roling, Luke T., and Abild-Pedersen, Frank. Sun . "Structure-Sensitive Scaling Relations: Adsorption Energies from Surface Site Stability". United States. doi:10.1002/cctc.201701841. https://www.osti.gov/servlets/purl/1457171.
@article{osti_1457171,
title = {Structure-Sensitive Scaling Relations: Adsorption Energies from Surface Site Stability},
author = {Roling, Luke T. and Abild-Pedersen, Frank},
abstractNote = {Here, the design of heterogeneous catalysts is accelerated by the identification of thermochemical reactivity descriptors, which enable the prediction of promising materials through efficient screening. Motivated by previous discoveries of linear scaling relations between the adsorption energies of related atoms and molecules, we present a new scaling between the adsorption energies of metal atoms and metal–adsorbate complexes, which can be used to directly predict catalytically relevant molecular adsorption energies. In contrast to existing models based on the coordination number of surface atoms alone, our model can predict adsorption energies with site–by–site resolution considering local structural effects and also has potential extensions to include contributions of neighboring metal identity in alloy systems. Integration of this scaling with a previously identified model for metal–metal interactions enables the accurate prediction of molecular adsorption energies on nanoparticles by performing only a small set of slab–based calculations.},
doi = {10.1002/cctc.201701841},
journal = {ChemCatChem},
issn = {1867-3880},
number = 7,
volume = 10,
place = {United States},
year = {2017},
month = {12}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

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Cited by: 6 works
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Figures / Tables:

Figure 1. Figure 1.: Adsorption structures for determination of ∆𝐸𝑀−𝐶𝑂 and ∆𝐸𝐶𝑂. An adsorbate molecule binds atop a metal atom (blue) with varying coordination number (CN) to other metal atoms (grey): (A) CN=3, fcc(111); (B) CN=5, fcc(111); (C) CN=7, fcc(111); (D) CN=9, fcc(111); (E) CN=4, fcc(100); (F) CN=4, fcc(100); (G) CN=6, fcc(100);more » (H) CN=6, fcc(100); (I) CN=8, fcc(100); (J) CN=8, fcc(100); (K) CN=5, fcc(211); (L) CN=6, fcc(211); (M) CN=7, fcc(211). Other atom colors: O (red), C (black).« less

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.