Antiferroelectric SnO₂ Network with Amorphous Surface for Electrochemical N₂ Fixation

Abstract

AbstractElectrochemical nitrogen fixation‐a sustainable pathway for converting abundant N2 into NH3 using renewable energy‐holds transformative potential for revolutionizing artificial nitrogen cycles. Nevertheless, even the state‐of‐the‐art catalytic systems also suffer from inadequate N2 adsorption capacity, which critically limits ammonia production rates and Faradaic efficiency (FE). To overcome this bottleneck, we strategically leveraged the antiferroelectric properties of SnO2 to establish dipole–dipole interactions with N2 molecules, synergistically enhancing both N2 adsorption and activation kinetics. Building on this foundation, we construct a three‐dimensional (3D) porous SnO2 network with unsaturated amorphous surfaces. Both experiment and first‐principles calculations indicate that all the exposed antiferroelectric surfaces could effectively adsorb N2, enhancing the N2 adsorption ability and maximizing active sites accessibility. The optimized catalyst delivers exceptional performance, achieving an NH3 production rate of 57.38 µg h−1mg−1cat 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.