Improved Representations of Heterogeneous Carbon Reforming Catalysis Using Machine Learning

Title
Improved Representations of Heterogeneous Carbon Reforming Catalysis Using Machine Learning
Publication Date
2019-10-15
Author(s)
Li, Xinyu
Chiong, Raymond
( author )
OrcID: https://orcid.org/0000-0002-8285-1903
Email: rchiong@une.edu.au
UNE Id une-id:rchiong
Hu, Zhongyi
Cornforth, David
Page, Alister J
Type of document
Journal Article
Language
en
Entity Type
Publication
Publisher
American Chemical Society
Place of publication
United States of America
DOI
10.1021/acs.jctc.9b00420
UNE publication id
une:1959.11/61433
Abstract

Predicting adsorption energies of reaction intermediates is critical for determining catalytic reaction mechanisms. Here, we present three combined representations for predicting adsorption energies of carbon reforming species on transition-metal surfaces. Among the three combined representations, the Elemental Properties and Spectral London Axilrod−Teller−Muto (EP&SLATM) representation, which uses separate EP and SLATM representations for the surface and adsorbates, yields the lowest mean absolute error (MAE) of ∼0.18 eV with respect to density functional theory (DFT) adsorption formation energies for 68 adsorbates on four low-index metal facets (Cu(111), Pt(111), Pd(111), Ru(0001)).All three combined representations also have lower MAEs compared with linear scaling relations. Notably, two of the combined representations achieve their results using empirical/experimental molecular structures only (i.e., without recourse to structural optimization based on first-principles methods such as DFT). The combined representations enable improved efficiency for predicting heterogeneous catalytic mechanisms using machine learning approaches, largely bypassing expensive electronic structure calculations. Further, we show that the combined representations enable "cross-surface" training with regression and tree-based machine learning methods. That is, to predict adsorption formation energies on a particular catalyst metal, these methods only need a small amount of training samples (20%) on that metal.

Link
Citation
Journal of Chemical Theory and Computation, 15(12), p. 6882-6894
ISSN
1549-9626
1549-9618
Start page
6882
End page
6894

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