Abstract
We present a novel “structure upgrading” synthetic approach for the design and synthesis of bio-inspired hydrogen-evolving electrocatalysts based on Cu-doped g-C3N4.
•“Structure upgrading” synthesis leads to hydrogen-evolving electrocatalysts.•Electrocatalysts based on earth-abundant elements was demonstrated.•Cu-doped g-C3N4 electrocatalyzes hydrogen evolution reaction (HER).•Bioinspired Cu-doped g-C3N4 has modest overpotentials for HER.•Cu-doped g-C3N4 shows good stability for HER in aqueous media.
Splitting water effectively to produce hydrogen (H2) requires the development of non-noble-metal electrocatalysts that are able to make this reaction feasible and energy efficient. Herein, we present a novel “structure upgrading” synthetic approach for the design and synthesis of bio-inspired hydrogen-evolving electrocatalysts based on earth-abundant elements. Using g-C3N4 – an inexpensive inorganic polymer material – as a host material for copper ions, novel Cu-doped g-C3N4 materials with supramolecular structure, efficient electrocatalytic activity and modest overpotentials for hydrogen evolution reaction (HER) are synthesized. Compared with most single-molecule analogs of hydrogenases that work only in organic media, the supramolecular Cu-doped g-C3N4 materials can serve as heterogeneous electrocatalysts with greater stability and good catalytic activity for HER in aqueous media. The materials afford a current density as high as 10mAcm−2 at an overpotential as low as 390mV, and work well in acidic media for, at least, 43h.