期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 10, 期 18, 页码 5381-5386出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.9b01460
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资金
- NSFC [21503257, 21601198]
- SinoDanish Centre (SDC)
- Villum Foundation Young Investigator Programme [VKR023449]
- Danish National Research Foundation (Carbon Dioxide Activation Center) [DNRF 118]
- Carlsberg Foundation
- Synfuels China Technology Co. Ltd.
Solar-driven production of renewable energy (e.g., H-2) has been investigated for decades. To date, the applications are limited by low efficiency due to rapid charge recombination (both radiative and nonradiative modes) and slow reaction rates. Tremendous efforts have been focused on reducing the radiative recombination and enhancing the interfacial charge transfer by engineering the geometric and electronic structure of the photocatalysts. However, fine-tuning of nonradiative recombination processes and optimization of target reaction paths still lack effective control. Here we show that minimizing the nonradiative relaxation and the adsorption energy of photogenerated surface-adsorbed hydrogen atoms are essential to achieve a longer lifetime of the charge carriers and a faster reaction rate, respectively. Such control results in a 16-fold enhancement in photocatalytic H-2 evolution and a 15-fold increase in photocurrent of the crystalline g-C3N4 compared to that of the amorphous g-C3N4.
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