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Engineering the Coordination Environment of Single-Atom Platinum Anchored on Graphdiyne for Optimizing
Xue-Peng Yin1, Hong-Juan Wang1, Shang-Feng Tang1
1Institute for New Energy Materials & Low Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin, 300384, China.
Abstract:
Two Pt single-atom catalysts (SACs) of Pt-GDY1 and Pt-GDY2 were prepared on graphdiyne (GDY)supports. The isolated Pt atoms are dispersed on GDY through the coordination interactions between Pt atoms and alkynyl C atoms in GDY, with the formation of five-coordinated C1 -Pt-Cl4 species in Pt-GDY1 and four-coordinated C2 -Pt-Cl2 species in Pt-GDY2. Pt-GDY2 shows exceptionally high catalytic activity for the hydrogen evolution reaction (HER), with a mass activity up to 3.3 and 26.9 times more active than Pt-GDY1 and the state-of-the-art commercial Pt/C catalysts, respectively. Pt-GDY2 possesses higher total unoccupied density of states of Pt 5d orbital and close to zero value of Gibbs free energy of the hydrogen adsorption (|ΔGPtH* |) at the Pt active sites, which are responsible for its excellent catalytic performance. This work can help better understand the structure-catalytic activity relationship in Pt SACs.
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