A ball-milling synthesis of N-graphyne with controllable nitrogen doping sites for efficient electrocatalytic oxygen evolution and supercapacitors

Abstract

Low-cost and efficient multifunctional electrodes play an important part in promoting the practical application of energy conversion and storage. Herein, we report the facile synthesis of N-graphyne, with a novel structure, by one-step ball milling of CaC₂ and pyrazine. The accurate doping of nitrogen atoms at the controllable sites of the molecular skeleton of γ-graphyne was achieved using the nitrogenous precursor (pyrazine) as a reactant. Various techniques were adopted for the investigation of the composition, structure, and morphology of the obtained samples. The electrochemical measurements demonstrated that N-graphyne can serve as an excellent electrode material for both electrocatalysis and supercapacitors. As an electrocatalyst, N-graphyne exhibited an overpotential of 280 mV at 100 mA cm⁻² and a Tafel slope of 122 mV dec⁻¹ for the oxygen evolution reaction with highly stable morphology and electrocatalytic performance. As a supercapacitor electrode, N-graphyne showed a maximum capacitance of 235 F g⁻¹ at 1 A g⁻¹, and capacitance retention of 87% after 3000 cycles. The superior electrochemical performance of N-graphyne is due to the nitrogen heteroatomic defects, large electrochemical active surface areas and fast electron migration. Our studies provide a facile synthesis of novel N-graphyne with controllable doping sites and promote its potential applications in electrocatalysis and supercapacitors.