Journal
ADVANCED MATERIALS
Volume 33, Issue 9, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202008180
Keywords
bottom-up strategies; high-concentration Ti3+; photocatalytic ammonia synthesis; porous carbon-doped TiOx nanosheets; visible light
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Funding
- NSFC [21575014, 21905025]
- Beijing Natural Science Foundation [2184122]
- Fundamental Research Funds for the Central Universities [2018CX01017]
- Beijing Institute of Technology Research Fund Program for Young Scholars
- State Key Laboratory of Explosion Science and Technology (Beijing Institute of Technology) [YBKT18-03]
- China Scholarship Council
- Analysis & Testing Center, Beijing Institute of Technology
- UK EPSRC [EP/N009533/1]
- Royal Society-Newton Advanced Fellowship Grant [NA170422]
- Leverhulme Trust [RPG-2017-122]
- EPSRC [EP/N009533/1] Funding Source: UKRI
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The study presents porous carbon-doped anatase TiOx (C-TiOx) nanosheets with high-concentration active sites of Ti3+ obtained through a reproducible bottom-up approach. It demonstrates that the high-concentration Ti3+ sites play a vital role in enhancing N-2 photoreduction activity. Combined with the morphology of porous nanosheets and the loading of a Ru/RuO2 cocatalyst, the optimized C-TiOx shows a high NH3 production rate and remarkable quantum efficiency under visible-light irradiation, outperforming current TiO2-based photocatalysts.
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 TiOx (C-TiOx) nanosheets with high-concentration active sites of Ti3+ are presented, which are produced by layered Ti3SiC2 through a reproducible bottom-up approach. It is shown that the high-concentration Ti3+ sites are the major species for the significant increase in N-2 photoreduction activity by the C-TiOx. Such bottom-up substitutional doping of C into TiO2 is responsible for both visible absorption and generation of Ti3+ concentration. Together with the porous nanosheets morphology and the loading of a Ru/RuO2 nanosized cocatalyst for enhanced charge separation and transfer, the optimal C-TiOx with a Ti3+/Ti4+ ratio of 72.1% shows a high NH3 production rate of 109.3 mu mol 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 TiO2-based photocatalysts at present.
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