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Abstract:
Catalytically active metals atomically dispersed on supports presents the ultimate atom utilization efficiency and cost-effective pathway for electrocatalyst design. Optimizing the coordination nature of metal atoms represents the advanced strategy for enhancing the catalytic activity and the selectivity of single-atom catalysts (SACs). Here, we designed a transition-metal based sulfide-Ni3S2 with abundant exposed Ni vacancies created by the interaction between chloride ions and the functional groups on the surface of Ni3S2 for the anchoring of atomically dispersed Pt (Pt-SA-Ni3S2). The theoretical calculation reveals that unique Pt-Ni3S2 support interaction increases the d orbital electron occupation at the Fermi level and leads to a shift-down of the d -band center, which energetically enhances H2O adsorption and provides the optimum H binding sites. Introducing Pt into Ni position in Ni3S2 system can efficiently enhance electronic field distribution and construct a metallic-state feature on the Pt sites by the orbital hybridization between S-3p and Pt-5d for improved reaction kinetics. Finally, the fabricated Pt-SA-Ni3S2 SAC is supported by Ag nanowires network to construct a seamless conductive three-dimensional (3D) nanostructure (Pt-SA-Ni3S2@Ag NWs), and the developed catalyst shows an extremely great mass activity of 7.6 A mg(-1) with 27-time higher than the commercial Pt/C HER catalyst.
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ADVANCED SCIENCE
Year: 2021
Issue: 12
Volume: 8
1 5 . 1 0 0
JCR@2022
JCR Journal Grade:1
Cited Count:
WoS CC Cited Count: 64
SCOPUS Cited Count: 65
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 11
Affiliated Colleges: