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

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America

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.

Research Organization:
Univ. of Rochester, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF)
Grant/Contract Number:
SC0002106; FG02-09ER16121; CBET-1437656
OSTI ID:
1540267
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Vol. 114, Issue 43; ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 41 works
Citation information provided by
Web of Science

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Semiconducting quantum dots for artificial photosynthesis journal July 2018
Stable p‐type Cu:CdS 1− x Se x /Pt Thin‐Film Photocathodes with Fully Tunable Bandgap for Scavenger‐Free Photoelectrochemical Water Splitting journal January 2020
Recent Advances in Sensitized Photocathodes: From Molecular Dyes to Semiconducting Quantum Dots journal January 2018
Energy transfer-enhanced photocatalytic reduction of protons within quantum dot light-harvesting–catalyst assemblies journal August 2018
Quantum Dot Assembly for Light-Driven Multielectron Redox Reactions, such as Hydrogen Evolution and CO 2 Reduction journal May 2019
Semiconductor Quantum Dots: An Emerging Candidate for CO 2 Photoreduction journal June 2019
ZnSe Nanorods as Visible‐Light Absorbers for Photocatalytic and Photoelectrochemical H 2 Evolution in Water journal March 2019
Hybrid Photoelectrochemical Water Splitting Systems: From Interface Design to System Assembly journal June 2019