期刊
NANO LETTERS
卷 18, 期 9, 页码 5954-5960出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.8b02740
关键词
Charge separation; graphitic carbon nitride; photoanode; porous nanorod array; solar water splitting; exciton dissociation
类别
资金
- National Natural Science Foundation of China [21422303, 21573049]
- National Key R&D Program nanotechnology special focus [2016YFA0201600]
- Beijing Natural Science Foundation [2142036]
- Knowledge Innovation Program
- Youth Innovation Promotion Association
- Special Program of One Belt One Road of CAS
Because of inefficient charge utilization caused by localized pi-electron conjugation and large exciton binding energy, the photoelectrochemical water-splitting efficiency of organic polymers is seriously limited. Taking the graphitic carbon nitride (g-CN) polymer as an example, we report a novel photoanode based on a vertically aligned g-CN porous nanorod (PNR) array prepared in situ, using a thermal polycondensation approach, with anodic aluminum oxide as the template. The g-CN PNR array exhibits an excellent photocurrent density of 120.5 mu A cm(-2) at 1.23 V-RHE under one sun illumination, the highest reported incident photon-to-current efficiency of similar to 15% at 360 nm, and an outstanding oxygen evolution reaction stability in 0.1 M Na2SO4 aqueous solution, which constitutes a benchmark performance among the reported g-CN-based polymer photoanodes without any sacrificial reagents. When compared with its planar counterpart, the enhanced performance of the PNR array results principally from its unique structure that enables a high degree of aromatic ring pi-electron conjugation for higher mobility of charge carriers, provides a direct pathway for the electron transport to the substrate, produces a large portion of hole-accepting defect sites and space charge region to promote exciton dissociation, and also withstands more strain at the interface to ensure intimate contact with the substrate. This work opens a new avenue to develop nanostructured organic semiconductors for large-scale application of solar energy conversion devices.
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