Activating MoS 2 Basal Plane with Ni 2 P Nanoparticles for Pt‐Like Hydrogen Evolution Reaction in Acidic Media

2D molybdenum disulfide (MoS 2 ) displays a modest hydrogen evolution reaction (HER) activity in acidic media because the active sites are limited to a small number of edge sites with broader basal planes remaining mostly inert. Here, it is reported that the MoS 2 basal planes could be activated by growing nickel phosphide (Ni 2 P) nanoparticles on them. Thus a Ni 2 P/MoS 2 heterostructure is constructed via in situ phosphidation of an indigenously synthesized NiMoS 4 salt as a single precursor to form a widely cross‐doped and chemically connected heterostructure. The conductivity and stability of the Ni 2 P/MoS 2 heterostructure are further enhanced by hybridization with conductive N‐doped carbon supports. As a result, the Ni 2 P/MoS 2 /N:RGO or Ni 2 P/MoS 2 /N:CNT electrocatalyst displays Pt‐like HER performance in acidic media, outperforming the incumbent best HER electrocatalyst, Pt/C, in a more meaningful high current density region (>200 mA cm −2 ) making them a promising candidate for practical water electrolysis applications. Since nonprecious metal catalysts showing Pt‐like HER performance in acidic media are rare, the Ni 2 P/MoS 2 heterostructure catalyst is a promising candidate for practical hydrogen production via water electrolysis.