Antiferroelectric SnO2 Network with Amorphous Surface for Electrochemical N2 Fixation

Abstract Electrochemical nitrogen fixation‐a sustainable pathway for converting abundant N 2 into NH 3 using renewable energy‐holds transformative potential for revolutionizing artificial nitrogen cycles. Nevertheless, even the state‐of‐the‐art catalytic systems also suffer from inadequate N 2 adsorption capacity, which critically limits ammonia production rates and Faradaic efficiency (FE). To overcome this bottleneck, we strategically leveraged the antiferroelectric properties of SnO 2 to establish dipole–dipole interactions with N 2 molecules, synergistically enhancing both N 2 adsorption and activation kinetics. Building on this foundation, we construct a three‐dimensional (3D) porous SnO 2 network with unsaturated amorphous surfaces. Both experiment and first‐principles calculations indicate that all the exposed antiferroelectric surfaces could effectively adsorb N 2 , enhancing the N 2 adsorption ability and maximizing active sites accessibility. The optimized catalyst delivers exceptional performance, achieving an NH 3 production rate of 57.38 µg h −1 mg −1 cat and a FE of 33.26%, representing one of the highest reported values among aqueous‐phase ammonia synthesis catalysts. These breakthroughs not only establish a universal design framework for gas‐involving electrocatalysts but also pioneer an integrated strategy to elevate nitrogen utilization efficiency in next‐generation sustainable energy infrastructures.