Graphdiyne (GDY), a novel large π-conjugated carbon material, for the first time, is introduced as the hole transfer layer into photoelectrochemical water splitting cell (PEC). Raman and ultraviolet photoelectron spectroscopic studies indicate the existence of relative strong π-π interactions between GDY and 4-mercaptopyridine surface-functionalized CdSe QDs, beneficial to the hole transportation and enhancement of the photocurrent performance. Upon exposure to 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 hours. All of the results indicate that GDY is a promising hole transfer material to fabricate PEC device for water splitting by solar energy. crucial step for PEC water splitting. Therefore, developing suitable photocathode materials with advantage of high hole mobility, appropriate valence band position, ease of fabrication and high stability, is the key to improve the PEC performance and stability.

J. Am. Chem. Soc., Just Accepted Manuscript ? DOI: 10.1021/jacs.5b12758 ? Publication Date (Web): 10 Mar 2016

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