Martin, DJ; Qiu, K; Shevlin, SA; Handoko, AD; Chen, X; Guo, Z; Tang, J; (2014) Highly Efficient Photocatalytic H2 Evolution from Water using Visible Light and Structure-Controlled Graphitic Carbon Nitride. Angew Chem Int Ed Engl , 53 (35) pp. 9240-9245. 10.1002/anie.201403375.

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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-C3 N4 ) from a low-cost precursor, urea, is reported. The g-C3 N4 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-C3 N4 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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