Journal
ADVANCED MATERIALS
Volume 31, Issue 16, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201806482
Keywords
N-2 fixation; oxygen vacancies; photocatalysis; TiO2; ultrathin nanosheets
Categories
Funding
- National Key Projects for Fundamental Research and Development of China [2017YFA0206904, 2017YFA0206900, 2016YFB0600901]
- National Natural Science Foundation of China [51825205, 51772305, 51572270, U1662118, 21871279, 21802154]
- Beijing Natural Science Foundation [2191002, 2182078, 2194089]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17000000]
- Royal Society-Newton Advanced Fellowship [NA170422]
- International Partnership Program of Chinese Academy of Sciences [GJHZ1819]
- Beijing Municipal Science and Technology Project [Z181100005118007]
- K. C. Wong Education Foundation
- Young Elite Scientist Sponsorship Program by CAST (YESS)
- Youth Innovation Promotion Association of the CAS
- Energy Education Trust of New Zealand
- MacDiarmid Institute for Advanced Materials and Nanotechnology
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Dinitrogen reduction to ammonia using transition metal catalysts is central to both the chemical industry and the Earth's nitrogen cycle. In the Haber-Bosch process, a metallic iron catalyst and high temperatures (400 degrees C) and pressures (200 atm) are necessary to activate and cleave NN bonds, motivating the search for alternative catalysts that can transform N-2 to NH3 under far milder reaction conditions. Here, the successful hydrothermal synthesis of ultrathin TiO2 nanosheets with an abundance of oxygen vacancies and intrinsic compressive strain, achieved through a facile copper-doping strategy, is reported. These defect-rich ultrathin anatase nanosheets exhibit remarkable and stable performance for photocatalytic reduction of N-2 to NH3 in water, exhibiting photoactivity up to 700 nm. The oxygen vacancies and strain effect allow strong chemisorption and activation of molecular N-2 and water, resulting in unusually high rates of NH3 evolution under visible-light irradiation. Therefore, this study offers a promising and sustainable route for the fixation of atmospheric N-2 using solar energy.
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