Journal
ACS NANO
Volume 15, Issue 11, Pages 17820-17830Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.1c06017
Keywords
niobic acid; boron dopant; oxygen vacancy; photocatalyst; nitrogen photofixation
Categories
Funding
- National Natural Science Foundation of China [21972015, 22088102, 12074053]
- Young Top Talents Project of Liaoning Province [XLYC1907147, XLYC1907163]
- Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science [2019JH3/30100003]
- Fundamental Research Funds for the Central Universities [DUT20TD06]
- Liaoning Revitalization Talent Program [XLYC2008032]
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This study reports the efficient nitrogen photofixation using two-dimensional boron-doped niobic acid nanosheets with oxygen vacancies, achieving enhanced ammonia evolution rates under visible-light irradiation in pure water. The synergy of boron dopant and oxygen vacancy plays a crucial role in regulating the band structure of niobic acid, facilitating charge transfer, reducing energy barriers, and promoting high rates of ammonia evolution, providing a general strategy for designing active photocatalysts for solar nitrogen conversion.
Direct nitrogen photofixation is a feasible solution toward sustainable production of ammonia under mild conditions. However, the generation of active sites for solar-dirven nitrogen fixation not only limits the fundamental understanding of the relationship among light absorption, charge transfer, and catalytic efficiency but also influences the photocatalytic activity. Herein, we report two-dimensional boron-doped niobic acid nanosheets with oxygen vacancies (B-V-o-HNbO3 NSs) for efficient N-2 photofixation in the absence of any scavengers and cocatalysts. Impressively, B-V-o-HNbO3 NS as a model catalyst achieves the enhanced ammonia evolution rate of 170 mu mol g(cat)(-1) h(-1) in pure water under visible-light irradiation. The doublet coupling representing (NH4+)-N-15 in an isotopic labeling experiment and in situ infrared spectra confirm the reliable ammonia generation. The experimental analysis and density functional theory (DFT) calculations indicate that the strong synergy of boron dopant and oxygen vacancy regulates band structure of niobic acid, facilitates photogenerated charge transfer, reduces free energy barriers, accelerates reaction kinetics, and promotes the high rates of ammonia evolution. This work provides a general strategy to design active photocatalysts toward solar N-2 conversion.
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