Abstract
The electrochemical nitrogen reduction reaction (NRR) provides a sustainable and alternative avenue to the Haber-Bosch process for ammonia (NH3) synthesis. Despite the great efforts made on catalysts and electrolytes, unfortunately, current NRR suffers from low selectivity due to the overwhelming competition with the hydrogen evolution reaction (HER). Here, we present an adjusted three-phase interface to enhance nitrogen (N2) coverage on a catalyst surface and achieve a record-high Faradic efficiency (FE) up to 97% in aqueous solution. The almost entirely suppressed HER process combined with the enhanced NRR activity, benefiting from the efficient three-interface contact line, is responsible for the excellent selectivity toward NH3, as evidenced by the theoretical and experimental results. Our strategy also demonstrates the applicability to other catalysts that feature strong H adsorption ability, to boost the FE for NH3 synthesis above 90% and to improve the NRR activity by engineering the catalysts.