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Greatly Improving Electrochemical N 2 Reduction over TiO 2 Nanoparticles by Iron Doping

作者:Tongwei Wu, Xiaojuan Zhu, Zhe Xing, Shiyong Mou, Chengbo Li, Yanxia Qiao, Qian Liu, Yonglan Luo, Xifeng Shi, Yanning Zhang, Xuping Sun · 发表于:Angewandte Chemie International Edition · 年份:2019 · DOI:10.1002/anie.201911153 · 被引用次数:501 · 研究领域:Ammonia Synthesis and Nitrogen Reduction、Advanced Photocatalysis Techniques、Hydrogen Storage and Materials

Abstract Titanium‐based catalysts are needed to achieve electrocatalytic N 2 reduction to NH 3 with a large NH 3 yield and a high Faradaic efficiency (FE). One of the cheapest and most abundant metals on earth, iron, is an effective dopant for greatly improving the nitrogen reduction reaction (NRR) performance of TiO 2 nanoparticles in ambient N 2 ‐to‐NH 3 conversion. In 0.5 m LiClO 4 , Fe‐doped TiO 2 catalyst attains a high FE of 25.6 % and a large NH 3 yield of 25.47 μg h −1 mg cat −1 at −0.40 V versus a reversible hydrogen electrode. This performance compares favorably to those of all previously reported titanium‐ and iron‐based NRR electrocatalysts in aqueous media. The catalytic mechanism is further probed with theoretical calculations.