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Carbon-Defect-Driven Electroless Deposition of Pt Atomic Clusters for Highly Efficient Hydrogen Evolution
journal contribution
posted on 2020-03-13, 17:34 authored by Qingqing Cheng, Chuangang Hu, Guoliang Wang, Zhiqing Zou, Hui Yang, Liming DaiPt atomic clusters (Pt-ACs) display
outstanding electrocatalytic
performance because of their unique electronic structure with a large
number of highly exposed surface atoms. However, the small size and
large specific surface area intrinsically associated with ACs pose
challenges in the synthesis and stabilization of Pt-ACs without agglomeration.
Herein, we report a novel one-step carbon-defect-driven electroless
deposition method to produce ultrasmall but well-defined and stable
Pt-ACs supported by defective graphene (Pt-AC/DG) structures. A theoretical
simulation clearly revealed that the defective regions with a lower
work function and hence a higher reducing capacity compared to those
of normal hexagonal sites triggered the reduction of Pt ions preferentially
at the defect sites. Moreover, the strong binding energy between Pt
and carbon defects effectively restricted the migration of spontaneously
reduced Pt atoms to immobilize/stabilize the resultant Pt-ACs. Electrochemical
analyses demonstrated the high performance of Pt-ACs in catalyzing
the hydrogen evolution reaction, showing a greatly enhanced mass activity,
a high Pt utilization efficiency, and excellent stability compared
with commercial Pt/C catalysts. The integration of proton exchange
membrane water electrolysis with Pt-AC/DG as a cathode exhibited an
excellent hydrogen generation activity and extraordinary stability
(during 200 h of electrolysis) with a greatly reduced Pt usage compared
with commercial Pt/C catalysts.
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surface areaPt utilization efficiencymass activitybinding energyPt usagedefect siteshydrogen evolution reactionPt ionsPt Atomic Clusterswork function200 hcarbon defectsElectrochemical analyseshydrogen generation activityelectrocatalytic performanceACCarbon-Defect-Driven Electroless DepositionPt-ACproton exchange membrane water electrolysiscarbon-defect-driven electroless deposition methodsurface atomsEfficient Hydrogen Evolution PtPt atoms
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