Han, Q; Wu, C; Jiao, H; Xu, R; Wang, Y; Xie, J; Guo, Q; Han, Q; Wu, C; Jiao, H; Xu, R; Wang, Y; Xie, J; Guo, Q; Tang, J; - view fewer (2021) Rational Design of High‐Concentration Ti³⁺ in Porous Carbon‐Doped TiO₂ Nanosheets for Efficient Photocatalytic Ammonia Synthesis. Advanced Materials , 33 (9) , Article 2008180. 10.1002/adma.202008180.

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Abstract

Photocatalytic ammonia synthesis is exciting but quite challenging with a very moderate yield at present. One of the greatest challenges is to develop highly active centers in a photocatalyst for N_{2} reduction under ambient conditions. Herein, porous carbon‐doped anatase TiO_{x} (C‐TiO_{x}) nanosheets with high‐concentration active sites of Ti^{3+} are presented, which are produced by layered Ti_{3}SiC_{2} through a reproducible bottom‐up approach. It is shown that the high‐concentration Ti^{3+} sites are the major species for the significant increase in N2 photoreduction activity by the C‐TiO_{x}. Such bottom‐up substitutional doping of C into TiO_{2} is responsible for both visible absorption and generation of Ti^{3+} concentration. Together with the porous nanosheets morphology and the loading of a Ru/RuO_{2} nanosized cocatalyst for enhanced charge separation and transfer, the optimal C‐TiO_{x} with a Ti^{3+}/Ti^{4+} ratio of 72.1% shows a high NH3 production rate of 109.3 µmol g^{−1} h^{−1} under visible‐light irradiation and a remarkable apparent quantum efficiency of 1.1% at 400 nm, which is the highest compared to all TiO_{2}‐based photocatalysts at present.

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