Few Layered N, P Dual-Doped Carbon-Encapsulated Ultrafine MoP Nanocrystal/MoP Cluster Hybrids on Carbon Cloth: An Ultrahigh Active and Durable 3D Self-Supported Integrated Electrode for Hydrogen Evolution Reaction in a Wide pH Range

Development of highly active and stable electrocatalysts is a key to realize efficient hydrogen evolution through water electrolysis. Here, the development of a 3D self-supported integrated electrode constituting few layered N, P dual-doped carbon-encapsulated ultrafine MoP nanocrystal/MoP cluster hybrids on carbon cloth (FLNPC@MoP-NC/MoP-C/CC) is demonstrated. Benefiting from novel structural features including fully open and accessible nanoporosity, ultrasmall size of MoP-NCs on MoP-Cs as well as strong synergistic effects of N, P dual-doped carbon layers with MoP-NCs, the FLNPC@MoP-NC/MoP-C/CC as a 3D self-supported binder-free integrated electrode exhibits extraordinary catalytic activity for the hydrogen evolution reaction (HER) with extremely low overpotentials at all pH values ( j = 10 mA cm −2 at η = 74, 106, and 69 mV in 0.5 m H 2 SO 4 , 1.0 m PBS, and 1.0 m KOH electrolytes, respectively). To the best of our knowledge, the ultrahigh electrocatalytic performance represents one of the best MoP-based HER electrocatalysts reported so far. Additionally, few layered N, P dual-doped carbon can effectively prevent MoP-NC/MoP-C from corrosion, making the FLNPC@MoP-NC/MoP-C/CC exhibit nearly unfading stability after 50 h testing in acidic, neutral, and alkaline media, which shows great promise for electrocatalytic water splitting application.