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Highly Efficient Photocatalytic H 2 Evolution from Water using Visible Light and Structure‐Controlled Graphitic Carbon Nitride
Author(s) -
Martin David James,
Qiu Kaipei,
Shevlin Stephen Andrew,
Handoko Albertus Denny,
Chen Xiaowei,
Guo Zhengxiao,
Tang Junwang
Publication year - 2014
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201403375
Subject(s) - graphitic carbon nitride , photocatalysis , water splitting , hydrogen , carbon nitride , hydrogen production , nitride , quantum yield , visible spectrum , materials science , photochemistry , carbon fibers , polymerization , quantum efficiency , semiconductor , chemistry , catalysis , nanotechnology , polymer , optoelectronics , organic chemistry , composite number , physics , layer (electronics) , quantum mechanics , composite material , fluorescence
Abstract 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‐C 3 N 4 ) from a low‐cost precursor, urea, is reported. The g‐C 3 N 4 exhibits an extraordinary hydrogen‐evolution rate (ca. 20 000 μmol h −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‐C 3 N 4 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.