Graphdiyne: A Metal-Free Material as Hole Transfer Layer To Fabricate Quantum Dot-Sensitized Photocathodes for Hydrogen Production

• Published in: Journal of the American Chemical Society 2016-03, Vol.138 (12), p.3954-3957
• Main Authors: Li, Jian, Gao, Xin, Liu, Bin, Feng, Qingliang, Li, Xu-Bing, Huang, Mao-Yong, Liu, Zhongfan, Zhang, Jin, Tung, Chen-Ho, Wu, Li-Zhu
• Format: Article
• Language: English
• ISSN: 0002-7863; 1520-5126
• DOI: 10.1021/jacs.5b12758

Graphdiyne (GDY), a novel large π-conjugated carbon material, for the first time, is introduced as the hole transfer layer into a photoelectrochemical water splitting cell (PEC). Raman and ultraviolet photoelectron spectroscopic studies indicate the existence of relatively strong π–π interactions between GDY and 4-mercaptopyridine surface-functionalized CdSe quantum dots, beneficial to the hole transportation and enhancement of the photocurrent performance. Upon exposure to a Xe lamp, the integrated photocathode produces a current density of nearly −70 μA cm–2 at a potential of 0 V vs NHE in neutral aqueous solution. Simultaneously, the photocathode evolves H2 with 90 ± 5% faradic efficiency over three times and exhibits good stability within 12 h. All of the results indicate that GDY is a promising hole transfer material to fabricate a PEC device for water splitting by solar energy.