Abstract
Electrochemical synthesis of ammonia (NH(3)) in aqueous electrolyte has long been suffered from poor nitrogen (N(2)) supply owing to its low solubility and sluggish diffusion kinetics. Therefore, creating a N(2) rich microenvironment around catalyst surface may potentially improve the efficiency of nitrogen reduction reaction (NRR). Herein, a delicately designed N(2) filtering membrane consisted of polydimethylsiloxane is covered on catalyst surface via superspreading. Because this membrane let the dissolved N(2) molecules be accessible to the catalyst but block excess water, the designed N(2) rich microenvironment over catalyst leads to an optimized Faradaic efficiency of 39.4% and an NH(3) yield rate of 109.2 µg h(-1) mg(-1), which is superior to those of the most report metal-based catalysts for electrochemical NRR. This study offers alternative strategy for enhancing NRR performance.