“…[1] Currently,Ptbased catalysts are still the pioneering ones in catalyzing the hydrogen evolution reaction (HER), capable of working with greater efficiency irrespective of pH value; [2] however,t heir commercial applications are largely restricted by the highcost, scarce-reserve and unsatisfactory stability. [3] Seeking transition-metal-based electrocatalysts with cost-effective, earth-abundant, high-efficiency,a nd good durability thus is of significance to expedite global scalability of hydrogen energy applications. [4] To date,t ransition-metal for example, phosphides, [5] sulfides, [6] selenides, [7] nitrides, [3c, 8] borides, [9] and others, [10] have been explored to replace the Pt-based catalysts.A mong them, transition-metal phosphides (TMPs) have drawn attention, owing to the advantages they offer in terms of electrical conductivity,m echanical strength, chemical tolerance,and low cost.…”