4.8 Article

General Synthesis of Transition-Metal-Based Carbon-Group Intermetallic Catalysts for Efficient Electrocatalytic Hydrogen Evolution in Wide pH Range

Journal

ADVANCED ENERGY MATERIALS
Volume 12, Issue 20, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202200293

Keywords

DFT calculations; full water splitting; hydrogen evolution reaction; intermetallic compounds; metal silicides

Funding

  1. Natural Sciences and Engineering Research Council of Canada (NSERC)
  2. Institut National de la Recherche Scientifique (INRS)
  3. 111 Project [D20015]
  4. Fonds de Recherche du Quebec-Nature et Technologies (FRQNT)

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Alloying is an effective strategy for tuning the electronic structures of catalyst materials. Intermetallic compounds, with ordered atomic arrangements, provide a rich platform to study the relationships among chemical composition, atomic structure, electronic structure, and properties. In this study, a series of intermetallic compounds were synthesized through a facile method and demonstrated excellent catalytic activity and durability in the hydrogen evolution reaction.
Alloying is a well-accepted strategy for modulating the electronic structures of catalyst materials. Compared to disordered solid-solution alloys, intermetallic compounds feature ordered atomic arrangements and provide a unique platform with a rich and diverse resource to study the relationships among chemical composition, atomic structure, electronic structure, and properties. Unfortunately, it is still challenging to synthesize the nanostructures of intermetallic compounds for catalysis research. In this study, a series of intermetallic silicides (PtSi, RhSi, Ru2Si3, IrSi), germanide (Ru2Ge3), and stannides (Ru3Sn7, IrSn2, PdSn3, PdSn2) are rationally designed and constructed through a facile molten-salt-assisted route. As an example, the PtSi not only shows highly desirable electrocatalytic properties for the hydrogen evolution reaction (HER) with low overpotentials of 22, 38, and 66 mV at a current density of 10 mA cm(-2) in acidic, alkaline, and neutral media, respectively, but exhibits superior durability, as well as >97% faradic efficiency. The theoretical calculations suggest that the introduction of Si to Pt could weaken the binding energy between Pt and H atoms, which further facilitates the hydrogen generation during the HER process. Further, the findings inspired the authors to develop other kinds of metal-based carbon-group intermetallic phases with excellent activity in the HER and beyond.

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