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Nanomaterials
Volume 12
Issue 23
10.3390/nano12234309
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Article

The Local Coordination Effects on the Reactivity and Speciation of Active Sites in Graphene-Embedded Single-Atom Catalysts over Wide pH and Potential Range

by
Milica S. Ritopečki
1,
Ana S. Dobrota
1,
Natalia V. Skorodumova
2 and
Igor A. Pašti
1,*
1
University of Belgrade—Faculty of Physical Chemistry, Studentski trg 12-16, 11158 Belgrade, Serbia
2
Department of Materials Science and Engineering, School of Industrial Engineering and Management, KTH—Royal Institute of Technology, Brinellvägen 23, 100 44 Stockholm, Sweden
*
Author to whom correspondence should be addressed.
Nanomaterials 2022, 12(23), 4309; https://doi.org/10.3390/nano12234309
Submission received: 22 November 2022 / Revised: 29 November 2022 / Accepted: 30 November 2022 / Published: 5 December 2022
(This article belongs to the Special Issue Synthesis, Modification and Application of Graphene)
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Abstract

Understanding the catalytic performance of different materials is of crucial importance for achieving further technological advancements. This especially relates to the behaviors of different classes of catalysts under operating conditions. Here, we analyzed the effects of local coordination of metal centers (Mn, Fe, Co) in graphene-embedded single-atom catalysts (SACs). We started with well-known M@N4-graphene catalysts and systematically replaced nitrogen atoms with oxygen or sulfur atoms to obtain M@OxNy-graphene and M@SxNy-graphene SACs (x + y = 4). We show that local coordination strongly affects the electronic structure and reactivity towards hydrogen and oxygen species. However, stability is even more affected. Using the concept of Pourbaix plots, we show that the replacement of nitrogen atoms in metal coordinating centers with O or S destabilized the SACs towards dissolution, while the metal centers were easily covered by O and OH, acting as additional ligands at high anodic potentials and high pH values. Thus, not only should local coordination be considered in terms of the activity of SACs, but it is also necessary to consider its effects on the speciation of SAC active centers under different potentials and pH conditions.
Keywords: single-atom catalysts; graphene; activity; reactivity; stability; Pourbaix plots single-atom catalysts; graphene; activity; reactivity; stability; Pourbaix plots
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MDPI and ACS Style

Ritopečki, M.S.; Dobrota, A.S.; Skorodumova, N.V.; Pašti, I.A. The Local Coordination Effects on the Reactivity and Speciation of Active Sites in Graphene-Embedded Single-Atom Catalysts over Wide pH and Potential Range. Nanomaterials 2022, 12, 4309. https://doi.org/10.3390/nano12234309

AMA Style

Ritopečki MS, Dobrota AS, Skorodumova NV, Pašti IA. The Local Coordination Effects on the Reactivity and Speciation of Active Sites in Graphene-Embedded Single-Atom Catalysts over Wide pH and Potential Range. Nanomaterials. 2022; 12(23):4309. https://doi.org/10.3390/nano12234309

Chicago/Turabian Style

Ritopečki, Milica S., Ana S. Dobrota, Natalia V. Skorodumova, and Igor A. Pašti. 2022. "The Local Coordination Effects on the Reactivity and Speciation of Active Sites in Graphene-Embedded Single-Atom Catalysts over Wide pH and Potential Range" Nanomaterials 12, no. 23: 4309. https://doi.org/10.3390/nano12234309

APA Style

Ritopečki, M. S., Dobrota, A. S., Skorodumova, N. V., & Pašti, I. A. (2022). The Local Coordination Effects on the Reactivity and Speciation of Active Sites in Graphene-Embedded Single-Atom Catalysts over Wide pH and Potential Range. Nanomaterials, 12(23), 4309. https://doi.org/10.3390/nano12234309

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