Porous Flower-Like Nanoarchitectures Derived from Nickel Phosphide Nanocrystals Anchored on Amorphous Vanadium Phosphate Nanosheet Nanohybrids for Superior Overall Water Splitting

Transition metal phosphides (TMPs) and phosphates (TM-Pis) nanostructures are promising functional materials for energy storage and conversion. Nonetheless, controllable synthesis of crystalline/amorphous heterogeneous TMPs/TM-Pis nanohybrids or related nanoarchitectures remains challenging, and their electrocatalytic applications toward overall water splitting (OWS) are not fully explored. Herein, the Ni2P nanocrystals anchored on amorphous V-Pi nanosheet based porous flower-like nanohybrid architectures that are self-supported on carbon cloth (CC) substrate (Ni2P/V-Pi/CC) are fabricated by conformal oxidation and phosphorization of pre-synthesized NiV-LDH/CC. Due to the unique microstructures and strong synergistic effects of crystalline Ni2P and amorphous V-Pi components, the obtained Ni2P/V-Pi/CC owns abundant active sites, suitable surface/interface electronic structure and optimized adsorption-desorption of reaction intermediates, resulting in outstanding electrocatalytic performances toward hydrogen and oxygen evolution reactions in alkaline media. Correspondingly, the assembled Ni2P/V-Pi/CC||Ni2P/V-Pi/CC electrolyzer only needs an ultralow cell voltage (1.44 V) to deliver 10 mA cm-2 water-splitting currents, exceeding its counterparts, recently reported bifunctional catalysts-based devices, and Pt/C/CC||IrO2/CC pairs. Moreover, the Ni2P/V-Pi/CC||Ni2P/V-Pi/CC manifests remarkable stability. Also, such device shows a certain prospect for OWS in acidic media. This work may spur the development of TMPs/TMPis-based nanohybrid architectures by combining structure and phase engineering, and push their applications in OWS or other clean energy options. Porous flower-like nanoarchitectures derived from Ni2P nanocrystals/amorphous V-Pi nanosheet nanohybrids that self-supported on carbon cloth (CC) are developed for overall water-splitting. Due to the unique structure and strong coupling of crystalline/amorphous components, such Ni2P/V-Pi/CC only needs 1.44 V cell voltage for driving water-splitting to reach 10 mA cm-2 current, outperforming pure Ni2P/CC, V-Pi/CC, and recently reported bifunctional electrocatalysts.image