Issue 10, 2023

Single-atom catalysis enabled by high-energy metastable structures

Abstract

Owing to limited degrees of freedom, the active sites of stable single-atom catalyst (SAC) often have one structure that is energetically much lower than other local-minimum structures. Thus, the SAC adopts one lowest-energy structure (LES) with an overwhelmingly larger proportion than any other high-energy metastable structure (HEMS), and the LES is commonly assumed to be solely responsible for the catalytic performance of an SAC. Herein, we demonstrate with SACs anchored on CeO2 that the HEMS of an SAC, even though its proportion remains several orders of magnitude lower than the LES throughout the catalytic reaction, can dictate catalysis with extraordinary activity arising from its unique coordination environment and oxidation state. Thus, we unravel the key role of HEMS-enabled catalysis in single-atom catalysis, which shakes the common assumption in the studies of SACs and urges new developments in both experiment and theory to identify and exploit catalysis via HEMSs.

Graphical abstract: Single-atom catalysis enabled by high-energy metastable structures

Supplementary files

Article information

Article type
Edge Article
Submitted
20 dek 2022
Accepted
31 yan 2023
First published
01 fev 2023
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2023,14, 2631-2639

Single-atom catalysis enabled by high-energy metastable structures

Z. Xia, Y. Yin, J. Li and H. Xiao, Chem. Sci., 2023, 14, 2631 DOI: 10.1039/D2SC06962H

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