“…Therefore, it is an imperative but challenging task to construct highly-active noble-metal-free bifunctional electrocatalysts by coupling the efficient catalytic active species of HER with those of OER into one electrode controllably to achieve superior overall water splitting performances through their cooperative effects. [15][16][17] Two dimensional (2D) nanomaterials, including graphene, [18,19] black phosphorus (BP), [20] transition metal dichalcogenides, [21,22] hexagonal boron nitride, [23,24] metal-organic frameworks (MOFs), [25][26][27][28][29][30] MXenes, [31] and layered double hydroxides (LDHs), [32][33][34][35] etc, have attracted tremendous attention in the field of energy conversion and storage owing to their high surface areas and favorable electronic properties. Among them, LDHs are the most promising OER electrocatalysts to replace noble metals because of their low-cost, rich resources, and high intrinsic activities.…”