Nitrogen-Doped Graphene with a Three-Dimensional Architecture Assisted by Carbon Nitride Tetrapods as an Efficient Metal-Free Electrocatalyst for Hydrogen Evolution

Current polymer membrane-based electrolyzers use Pt as a cathode catalyst for efficient reduction of water. The high cost of Pt-based catalysts forces researchers to develop alternative electrocatalysts. Here, a simple strategy has been proposed to synthesize a metal-free electrocatalyst for the hydrogen evolution reaction (HER) by high-temperature annealing of graphene oxide-coated melamine foam. The prepared catalyst possesses both structural and functional advantages with its three-dimensional (3D) interconnected arms of carbon nitride (CNx) backbone wrapped with nitrogen-doped graphene (N-RGO) sheets (CNx@N-RGO). CNx@N-RGO faces only a 193 mV overpotential to achieve a current density of 10mAcm(-2), which is far superior to the previously reported Pt-free systems. Along with the high exchange current density 34.7 x 10(-6)A cm(-2) and low Tafel slope of 54 mV dec(-1), CNx@N-RGO follows a Volmer-Heyrovsky mechanism for the HER. DFT calculations show that the synergy between CNx and N-RGO facilitates good electrical coupling between the two moieties and provides optimal binding to H+ ions on the catalyst that, in turn, results in efficient reduction of hydrogen ions.