“…Particularly, hydrogen spillover has emerged as an effective contributor to overcome the limitation of the traditional Sabatier’s principle for further improving reaction kinetics during electrocatalytic hydrogen evolution reaction (HER). − To achieve the hydrogen spillover effect, binary metal–support electrocatalysts, consisting of an active component with a negative adsorption Gibbs free energy (Δ G H < 0) for strong intermediate adsorption and a support component with a positive energy (Δ G H > 0) for favorable hydrogen release, are required. , A representative example is loading noble-metal particles (e.g., Pt, Ru, Pd, and Ir), on a non-noble-metal-based support (e.g., MoS 2 , CoP, WO 3– x , TiO 2 , and CeO 2 ), which could induce the synergistic effects for hydrogen spillover and meanwhile reduce the utilization of high-cost noble metals without any obvious compromise on the catalytic performance. − For the metal component, platinum (Pt) has been intensively chosen as the active site due to the near-zero Δ G H . − Nevertheless, rational selection on the suitable support material remains elusive. In these pioneering reported metal–support HER catalysts, one-dimensional nanostructures (e.g., silicon wires) or two-dimensional nanosheets (e.g., MoS 2 and graphdiyne), were chosen as the support material. , For example, by the investigation on a series of Pt alloys and CoP catalysts, it was identified that a small work function difference between metal and support could cause the interfacial charge dilution and relocation, thus weakening interfacial proton adsorption and promoting hydrogen spillover for HER …”