Direct synthesis of nitrogen-rich carbon sheets via polybenzoxazine as highly active electrocatalyst for water splitting

In this work, we propose a novel nitrogen-rich carbon sheets (N-CSs), with conceivable use as efficient catalysts for hydrogen evolution reaction (HER). N-CSs are directly synthesized from polybenzoxazine (PBz) by carbonization followed by KOH activation. PBz was prepared from eugenol, melamine, and paraformaldehyde through ring-opening polymerization. FT-IR and NMR spectroscopy confirmed the corresponding chemical structures of the new benzoxazine monomer. The morphology, structure and surface properties of the N-CSs are investigated by Raman spectroscopy, wide-angle X-ray diffraction, and X-ray photoelectron spectroscopy. The catalytic activity of N-CSs towards HER is thoroughly investigated by electrochemical techniques. In N-CSs, it is established that nitrogen gratified electrocatalytic activity, and hence nitrogen atoms should enhance the electrocatalytic properties by increasing the active sites. As the kinetic current is stabilized by the outer nitrogen atom as such, HER is proposed to proceed on these active sites by the Volmer-Heyrovsky mechanism. The N-CSs show outstanding catalytic activity towards HER with lowest onset-potential (?10 mV_RHE) and Tafel slope (45 mV dec^?1) in 0.5 M H₂SO₄ aqueous electrolyte.