Self-supported electrocatalysts being generated and employed directly as electrodes for energy conversion has been intensively pursued in the fields of materials chemistry and energy. Herein, we report a synthetic strategy to prepare freestanding hierarchically structured, nitrogen-doped nanoporous graphitic carbon membranes functionalized with Janus-type Co/CoP nanocrystals (termed as HNDCM-Co/CoP), which were successfully applied as a highly efficient, binder-free electrode in the hydrogen evolution reaction (HER). Benefited from multiple structural merits, such as a high degree of graphitization, three-dimensionally interconnected micro/meso/macropores, uniform nitrogen doping, well-dispersed Co/CoP nanocrystals, as well as the confinement effect of the thin carbon layer on the nanocrystals, HNDCM-Co/CoP exhibited superior electrocatalytic activity and long-term operation stability for HER under both acidic and alkaline conditions. As a proof-of-concept of practical usage, a 5.6 cm × 4 cm × 60 μm macroscopic piece of HNDCM-Co/CoP was prepared in our laboratory. Driven by a solar cell, electroreduction of water in alkaline conditions (pH 14) was performed, and H was produced at a rate of 16 mL/min, demonstrating its potential as real-life energy conversion systems.
Bibliographical noteKAUST Repository Item: Exported on 2020-10-01
Acknowledgements: H.W. and T.W. thank the King Abdullah University of Science and Technology (KAUST) for financial support. S.M. acknowledges the financial support from the National Natural Science Foundation of China (21463001). J.Y. is grateful for financial support from the Max Planck Society, Germany, Clarkson University, USA, and the ERC (European Research Council) Starting Grant (Project Number 639720-NAPOLI).