Synergistic Contact‐Electro‐Catalysis and Photocatalysis via TiO 2 @PTFE Composites for Efficient N 2 to NH 3 Conversion

作者：Kaiyang Shi, Huan Meng, Jiajin Liu, Shuai Ma, Wei Tang · 发表于：Angewandte Chemie International Edition · 年份：2025 · DOI：10.1002/anie.202515707 · 被引用次数：23 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Advanced Photocatalysis Techniques、Caching and Content Delivery

Abstract Catalytic nitrogen fixation from N 2 and water under mild conditions offers a sustainable NH 3 synthesis route. Herein, we report a synergistic nitrogen fixation strategy combining contact‐electro‐catalysis (CEC) with photocatalysis via one‐step in situ hydrothermally synthesized TiO 2 @PTFE catalyst, and achieved an activity of 133.6 µmol g −1 h −1 . It represents 10.9‐fold and 7.5‐fold enhancements over pristine TiO 2 and PTFE, respectively, outperforming current CEC systems and many photocatalytic systems operating without sacrificial agents. Further characterization and theoretical calculations reveal the synergy: the composite catalyst enhances the CEC catalyst dispersion; the CEC‐generated electric fields promote photogenerated charge separation and elevate the semiconductor's Fermi level, bolstering photocatalytic N 2 reduction; conversely, the semiconductor boosts CEC efficiency via enhanced N 2 adsorption and supplemental electron donation. We anticipate that this work establishes a “two birds with one stone” strategy, providing novel insights into CEC‐photocatalysis synergy and a pathway for rational design of high‐performance nitrogen fixation catalysts.