Dual-Metal Hetero-Single-Atoms with Different Coordination for Efficient Synergistic Catalysis

Rationally tailoring the coordination environments of metal single atoms (SAs) is an effective approach to promote their catalytic performances, which, however, remains as a challenge to date. Here, we report a novel misplaced deposition strategy for the fabrication of differently coordinated dual-m...

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Veröffentlicht in:Journal of the American Chemical Society 2021-10, Vol.143 (39), p.16068-16077
Hauptverfasser: Zhao, Xin, Wang, Fengliang, Kong, Xiang-Peng, Fang, Ruiqi, Li, Yingwei
Format: Artikel
Sprache:eng
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Zusammenfassung:Rationally tailoring the coordination environments of metal single atoms (SAs) is an effective approach to promote their catalytic performances, which, however, remains as a challenge to date. Here, we report a novel misplaced deposition strategy for the fabrication of differently coordinated dual-metal hetero-SAs. Systematic characterization results imply that the as-synthesized dual-metal hetero-SAs (exemplified by Cu and Co) are affixed to a hierarchical carbon support via Cu–C4 and Co–N4 coordination bonds. Density functional theory studies reveal that the strong synergistic interactions between the asymmetrically deployed CuC4 and CoN4 sites lead to remarkably polarized charge distributions, i.e., electron accumulation and deficiency around CuC4 and CoN4 sites, respectively. The obtained CuC4/CoN4@HC catalyst exhibits significantly enhanced capability in substrate adsorption and O2 activation, achieving superior catalytic performances in the oxidative esterification of aromatic aldehydes in comparison with the Cu- and Co-based SA counterparts.
ISSN:0002-7863
1520-5126
DOI:10.1021/jacs.1c06349