LAUSR

Electrochemical ammonia (NH3) synthesis from nitrate (NO3-) reduction offers an intriguing approach for both sustainable ammonia synthesis and environmental denitrification, yet it remains hindered by a complicated reaction pathway with various intermediates. Here we present that the interlayer strain compression in bismuth (Bi) nanocrystals can contribute to both activity and selectivity improvement toward NH3 electrosynthesis from NO3- reduction. By virtue of comprehensive spectroscopic studies and theoretical calculations, we untangle that the interlayer lattice compression shortens Bi-Bi bond to broaden the 6p bandwidth for electron delocalization, promoting the chemical affinities of nitrogen intermediates. Such a manipulation facilitates NO3- activation to reduce the energy barrier for activity improvement, and also alleviates *NO2 desorption to suppress nitrite generation. As a result, a strain-compressive Bi electrocatalyst yields a maximal Faradaic efficiency of 90.6% and high generation rate of 46.5 g h-1 gcat-1 with industrially scalable partial current density up to 300 mA cm-2 for NH3 product at the optimized conditions, respectively.