期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 114, 期 43, 页码 11297-11302出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1712325114
关键词
photochemical; hydrogen; photocathode; semiconductor; quantum dot
资金
- Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, US Department of Energy [DE-FG02-09ER16121]
- National Science Foundation [CBET-1437656]
The present study reports the fabrication of CdSe quantum dot (QD)-sensitized photocathodes on NiO-coated indium tin oxide (ITO) electrodes and their H-2-generating ability upon light irradiation. A well-established spin-coating method was used to deposit CdSe QD stock solution onto the surface of NiO/ITO electrodes, thereby leading to the construction of various CdSe QD-sensitized photocathodes. The present report includes the construction of rainbow photocathodes by spin-coating different-sized QDs in a sequentially layered manner, thereby creating an energetically favorable gradient for charge separation. The resulting rainbow photocathodes with forward energetic gradient for charge separation and subsequent electron transfer to a solution-based hydrogen-evolving catalyst (HEC) exhibit good light-harvesting ability and enhanced photoresponses compared with the reverse rainbow photocathodes under white LED light illumination. Under minimally optimized conditions, a photocurrent density of as high as 115 mu A.cm(-2) and a Faradaic efficiency of 99.5% are achieved, which is among the most effective QD-based photocathode water-splitting systems.
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