Solving the structure of “single-atom” catalysts using machine learning – assisted XANES analysis

Xiang, Shuting; Huang, Peipei; Li, Junying; Liu, Yang; Marcella, Nicholas; Routh, Prahlad K.; Li, Gonghu; Frenkel, Anatoly I.

doi:10.1039/d1cp05513e

Title: Solving the structure of “single-atom” catalysts using machine learning – assisted XANES analysis

Journal Article · 03 February 2022 · Physical Chemistry Chemical Physics. PCCP

DOI: https://doi.org/10.1039/d1cp05513e · OSTI ID:1855095

^[1]; Huang, Peipei ^[2]; Li, Junying ^[1]; Liu, Yang ^[1]; Marcella, Nicholas ^[1]; Routh, Prahlad K. ^[1];

^[2];

^[3]

Stony Brook Univ., NY (United States)
Univ. of New Hampshire, Durham, NH (United States)
Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

We show that "single-atom” catalysts (SACs) have demonstrated excellent activity and selectivity in challenging chemical transformations such as photocatalytic CO₂ reduction. For heterogeneous photocatalytic SAC systems, it is essential to obtain sufficient information of their structure at the atomic level in order to understand reaction mechanisms. In this work, a SAC was prepared by grafting a molecular cobalt catalyst on a light-absorbing carbon nitride surface. Due to the sensitivity of the X-ray absorption near edge structure (XANES) spectra to subtle variances in the Co SAC structure in reaction conditions, different machine learning (ML) methods, including principal component analysis, K-means clustering, and neural network (NN), were utilized for in situ Co XANES data analysis. As a result, we obtained quantitative structural information of the SAC nearest atomic environment thereby extending the NN-XANES approach previously demonstrated for nanoparticles and size-selective clusters.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704

OSTI ID:: 1855095

Report Number(s):: BNL-222862-2022-JAAM

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 8 Vol. 24; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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