Defect‐Enhanced Low‐Temperature CO Oxidation on Graphene‐Supported Pt‐Au Nanoclusters

Defect‐Enhanced Low‐Temperature CO Oxidation on Graphene‐Supported Pt‐Au Nanoclusters Full article

Journal

Small
ISSN: 1613-6829 , E-ISSN: 1613-6810

Output data

Year: 2026, Article number : e75835, Pages count : 16 DOI: 10.1002/smll.75835

Tags

active site, adsorption, bimetallic strip, chemical physics, dispersity, graphene, molecular dynamics, nanoclusters

Authors

Chepkasov Ilya V. ^1,2 , Baidyshev Viktor S. ² , Radina Aleksandra D. ² , Lukanov Michail M. ² , Baturin Vladimir S. ³ , Lazarev Mikhail ⁴ , Ter‐Oganessian Nikita V. ⁵ , Galushko Alexey S. ⁶ , Khrizanforov Mikhail N. ⁶ , Ananikov Valentine P. ⁶ , Kvashnin Alexander G. ²

Affiliations

1	Bauman Moscow State Technical University Moscow Russian Federation
2	Skolkovo Institute of Science and Technology Moscow Russian Federation
3	CNRS‐Saint‐Gobain‐NIMS, IRL 3629, Laboratory for Innovative Key Materials and Structures (LINK) National Institute for Materials Science (NIMS) Tsukuba Ibaraki Japan
4	HSE University Moscow Russia
5	Institute of Physics Southern Federal University Rostov‐on‐Don Russian Federation
6	Zelinsky Institute of Organic Chemistry Russian Academy of Sciences Moscow Russian Federation

The catalytic properties of bimetallic nanoclusters are governed by a complex interplay between their size, composition, chemical ordering, and interaction with the support. Here, we perform a comprehensive data-driven computational study using the USPEX evolutionary algorithm for global structure prediction of Pt–Au nanoclusters (up to 24 atoms), followed by high-throughput screening for O and CO adsorption energy with MACE foundation model and simulations of chemical reactor. We combine about 12 000 density functional theory (DFT) calculations with a machine learning workflow that adds over 80 000 additional data points to enable extensive sampling of ground-state and metastable isomers. Our analysis reveals that adsorption energies are primarily determined by local atomic composition of the active site rather than by the precise global-minimum structure. Consequently, a representative set of low-energy isomers provides the same adsorption information as the most stable clusters, which is crucial for experiments where monodisperse samples are difficult to obtain. We further demonstrate that a graphene substrate with a single carbon monovacancy strongly anchors cluster, enhances O2 adsorption, and lowers CO oxidation barriers by activating traditionally inert Au atoms. Molecular dynamics simulations of CO saturation show that the supported cluster undergoes adsorption-induced reconstruction, with Pt atoms segregating to the surface, and that the support significantly alters the saturation profile compared to the free-standing cluster. This work establishes that rational design of bimetallic catalysts must take into account for local site chemistry, dynamic synergy with the support, and practical relevance of isomer ensembles.

Chepkasov I.V. , Baidyshev V.S. , Radina A.D. , Lukanov M.M. , Baturin V.S. , Lazarev M. , Ter‐Oganessian N.V. , Galushko A.S. , Khrizanforov M.N. , Ananikov V.P. , Kvashnin A.G.
Defect‐Enhanced Low‐Temperature CO Oxidation on Graphene‐Supported Pt‐Au Nanoclusters
Small. 2026. e75835 :1-16. DOI: 10.1002/smll.75835 WOS Scopus OpenAlex

Submitted:	Jun 26, 2026
Accepted:	Sep 9, 2026
Published online:	Sep 24, 2026

≡ Web of science:	WOS:001883785800001
≡ Scopus:	2-s2.0-105051576941
≡ OpenAlex:	W7214206711