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Title: Semiconductor quantum dot-sensitized rainbow photocathode for effective photoelectrochemical hydrogen generation

Abstract

We discuss the fabrication of CdSe quantum dot (QD)-sensitized photocathodes on NiO-coated indium tin oxide (ITO) electrodes and their H2-generating ability upon light irradiation. A well-established spin-coating approach 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 μA•cm–2and a Faradaic efficiency of 99.5% are achieved, which is among the most capable QD-based photocathode water-splitting systems.

Authors:
 [1];  [1];  [1];  [1]; ORCiD logo [1];  [1];  [1]
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  1. Univ. of Rochester, NY (United States)
Publication Date:
Research Org.:
Univ. of Rochester, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF)
OSTI Identifier:
1540267
Grant/Contract Number:  
SC0002106; FG02-09ER16121; CBET-1437656
Resource Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 114; Journal Issue: 43; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; photochemical; hydrogen; photocathode; semiconductor; quantum dot

Citation Formats

Lv, Hongjin, Wang, Congcong, Li, Guocan, Burke, Rebeckah, Krauss, Todd D., Gao, Yongli, and Eisenberg, Richard. Semiconductor quantum dot-sensitized rainbow photocathode for effective photoelectrochemical hydrogen generation. United States: N. p., 2017. Web. doi:10.1073/pnas.1712325114.
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Lv, Hongjin, Wang, Congcong, Li, Guocan, Burke, Rebeckah, Krauss, Todd D., Gao, Yongli, & Eisenberg, Richard. Semiconductor quantum dot-sensitized rainbow photocathode for effective photoelectrochemical hydrogen generation. United States. https://doi.org/10.1073/pnas.1712325114
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Lv, Hongjin, Wang, Congcong, Li, Guocan, Burke, Rebeckah, Krauss, Todd D., Gao, Yongli, and Eisenberg, Richard. Mon . "Semiconductor quantum dot-sensitized rainbow photocathode for effective photoelectrochemical hydrogen generation". United States. https://doi.org/10.1073/pnas.1712325114. https://www.osti.gov/servlets/purl/1540267.
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@article{osti_1540267,
title = {Semiconductor quantum dot-sensitized rainbow photocathode for effective photoelectrochemical hydrogen generation},
author = {Lv, Hongjin and Wang, Congcong and Li, Guocan and Burke, Rebeckah and Krauss, Todd D. and Gao, Yongli and Eisenberg, Richard},
abstractNote = {We discuss the fabrication of CdSe quantum dot (QD)-sensitized photocathodes on NiO-coated indium tin oxide (ITO) electrodes and their H2-generating ability upon light irradiation. A well-established spin-coating approach 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 μA•cm–2and a Faradaic efficiency of 99.5% are achieved, which is among the most capable QD-based photocathode water-splitting systems.},
doi = {10.1073/pnas.1712325114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 43,
volume = 114,
place = {United States},
year = {2017},
month = {10}
}
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https://doi.org/10.1073/pnas.1712325114
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