Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 53, Issue 35, Pages 9240-9245Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201403375
Keywords
graphitic carbon nitride; hydrogen production; polymerization; protonation; water splitting
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Funding
- ESPRC [EP/H046380/1, EP/G063176/1]
- STEPCAP [EP/G061785/1]
- Qatar National Research Fund under its National Priorities Research Program [NPRP 09-328-2-122]
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The major challenge of photocatalytic water splitting, the prototypical reaction for the direct production of hydrogen by using solar energy, is to develop low-cost yet highly efficient and stable semiconductor photocatalysts. Herein, an effective strategy for synthesizing extremely active graphitic carbon nitride (g-C3N4) from a low-cost precursor, urea, is reported. The g-C3N4 exhibits an extraordinary hydrogen-evolution rate (ca. 20 000 mu molh(-1)g(-1) under full arc), which leads to a high turnover number (TON) of over 641 after 6 h. The reaction proceeds for more than 30 h without activity loss and results in an internal quantum yield of 26.5% under visible light, which is nearly an order of magnitude higher than that observed for any other existing g-C3N4 photocatalysts. Furthermore, it was found by experimental analysis and DFT calculations that as the degree of polymerization increases and the proton concentration decreases, the hydrogen-evolution rate is significantly enhanced.
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