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Self-supported electrocatalysts being generated and employed directly aselectrode for energy conversion has been intensively pursued in the fields ofmaterials chemistry and energy. Herein, we report a synthetic strategy toprepare freestanding hierarchically structured, nitrogen-doped nanoporousgraphitic carbon membranes functionalized with Janus-type Co/CoP nanocrystals(termed as HNDCM-Co/CoP), which were successfully applied as ahighly-efficient, binder-free electrode in hydrogen evolution reaction (HER).Benefited from multiple structural merits, such as high degree ofgraphitization, three-dimensionally interconnected micro-/meso-/macropores,uniform nitrogen-doping, well-dispersed Co/CoP nanocrystals as well as theconfinement effect of the thin carbon layer on the nanocrystals, HNDCM-Co/CoPexhibited superior electrocatalytic activity and long-term operation stabilityfor HER under both acid and alkaline conditions. As a proof-of-concept ofpractical usage, a macroscopic piece of HNDCM-Co/CoP of 5.6 cm x 4 cm x 60 umin size was prepared in our laboratory. Driven by a solar cell,electroreduction of water in alkaline condition (pH 14) was performed, and H2has been produced at a rate of 16 ml/min, demonstrating its potential asreal-life energy conversion systems.

acs nano

Nitrogen-doped Nanoporous Carbon Membranes Functionalized with Co/CoP  Janus-type nanocrystals as Hydrogen Evolution Electrode in Both Acid and  Alkaline Environment