Metal‐Organic Frameworks Derived Multidimensional CoP/N, P‐Doped Carbon Architecture as an Efficient Electrocatalyst for Overall Water Splitting

Abstract Exploring highly efficient non‐noble‐metal‐based electrocatalysts for water electrocatalysis is vitally important to meet the requirement for future hydrogen energy. In this work, we report a simple metal‐organic‐frameworks‐based one‐step calcination route to the rational design of a multidimensional bifunctional electrocatalyst, constituting 0D CoP nanocrystals embedded in N, P‐doped binary carbon networks with 1D carbon hollow nanotube and 2D carbon porous nanosheet. The elaborate hierarchical architecture allows for high exposure of active sites and continuous electron/ion transport pathwaysf1.02. Together with the strong coupling effect between CoP and hybrid carbon matrices, the obtained electrocatalyst can efficiently catalyze both hydrogen and oxygen evolution reactions. Specifically, low overpotentials of 103 and 260 mV are needed to deliver H 2 ‐evolving current of 10 mA cm −2 and O 2 ‐evolving current of 30 mA cm −2 , respectively. Remarkably, an alkaline electrolyzer comprising this electrocatalyst drives 10 mA cm −2 at a low cell voltage of 1.54 V, outperforming the integrated benchmarking Pt/C+IrO 2 couple, along with steady durability. The current work introduces a new way of developing innovative transition metal phosphides/carbon nanostructures for electrocatalysis and other energy‐related applications.