Oxygen-regulated carbon quantum dots as an efficient metal-free electrocatalyst for nitrogen reduction

Abstract

An electrocatalytic nitrogen reduction reaction under ambient conditions provides a wonderful blueprint for the conversion of nitrogen to ammonia. However, current research on ammonia synthesis is mainly focused on metal-based catalysts. It is still a great challenge to realize the effective activation of N₂ on non-metallic catalysts. Herein, carbon quantum dots are reported to reduce dinitrogen to ammonia under ambient conditions. Benefiting from its numerous defect sites, this metal-free catalyst shows excellent catalytic performance in 0.1 M HCl with a faradaic efficiency of 17.59%. In addition, both experimental and theoretical results confirm that the catalytic performance of the catalyst can be improved by appropriately controlling the oxygen content of samples at different temperatures, and the utmost ammonia yield is 134.08 μg h⁻¹ mg⁻¹_cat., which is almost three times higher than that of a reported metal-free material. The proposed oxygen regulation provides a new method to optimize the surface properties of metal-free catalysts for ammonia synthesis.