Antiferroelectric SnO<sub>2</sub> Network with Amorphous Surface for Electrochemical N<sub>2</sub> Fixation
Xiangyu Chen, Shuning Lv, Zhaoyu Li, Hongfei Gu, Xiaoyi Sun, Qi Hu, Yong Zhao, Zhaoyu Li, Tianqi Guo, Jianxin Kang, Limin Liu, Lin Guo
Abstract
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.