论文列表
论文列表
Single-Atom High-Valent Fe(IV) for Promoted Photocatalytic Nitrogen Hydrogenation on Porous TiO2-SiO2
来源: | 作者:吴仕群 | 发布时间: 2021-03-26 | 297 次浏览 | 分享到:
Shiqun Wu, Ziyu Chen, Wenhui Yue, Shinya Mine, Takashi Toyao, Masaya Matsuoka, Xinguo Xi, Lingzhi Wang*, and Jinlong Zhang*
Cite this: ACS Catal. 2021, 11, XXX, 4362–4371
Publication Date:March 24, 2021
https://doi.org/10.1021/acscatal.1c00072
Synergistic nitrogen reduction and water oxidation process is significant to the photocatalytic fixation of nitrogen. However, the coupling mechanism remains ambiguous and lacks study. Herein, we report enhanced photocatalytic nitrogen fixation on single-atom Fe-modified macro-/mesoporous TiO2-SiO2 (Fe-T-S), with a high ammonia generation rate of 32 μmol g–1 h–1 without any sacrificial agent and cocatalysts. Experimental and theoretic calculation studies confirmed the formation of a photoinduced hole-trapping polaron on the Fe dopant, resulting in the high-valent Fe(IV) species. The single-atom Fe(IV) site is responsible for water oxidation and helps promote N2 hydrogenation on neighboring oxygen vacancy. This study explicitly unravels the key to achieve the coupling between photocatalytic N2 hydrogenation and water oxidation through a doping strategy and provides significant guidance for the rational design of photocatalysts for ammonia synthesis.