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      Interface induce growth of intermediate layer for bandgap engineering insights into photoelectrochemical water splitting

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          Abstract

          A model of interface induction for interlayer growing is proposed for bandgap engineering insights into photocatalysis. In the interface of CdS/ZnS core/shell nanorods, a lamellar solid solution intermediate with uniform thickness and high crystallinity was formed under interface induction process. Merged the novel charge carrier transfer layer, the photocurrent of the core/shell/shell nanorod (css-NR) array was significantly improved to 14.0 mA cm −2 at 0.0 V vs. SCE, nearly 8 times higher than that of the perfect CdS counterpart and incident photon to electron conversion efficiency (IPCE) values above 50% under AM 1.5G irradiation. In addition, this array photoelectrode showed excellent photocatalytic stability over 6000 s. These results suggest that the CdS/Zn 1−xCd xS/ZnS css-NR array photoelectrode provides a scalable charge carrier transfer channel, as well as durability, and therefore is promising to be a large-area nanostructured CdS-based photoanodes in photoelectrochemical (PEC) water splitting system.

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          Most cited references19

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          Electrochemical photolysis of water at a semiconductor electrode.

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            Nitrogen-doped ZnO nanowire arrays for photoelectrochemical water splitting.

            We report the rational synthesis of nitrogen-doped zinc oxide (ZnO:N) nanowire arrays, and their implementation as photoanodes in photoelectrochemical (PEC) cells for hydrogen generation from water splitting. Dense and vertically aligned ZnO nanowires were first prepared from a hydrothermal method, followed by annealing in ammonia to incorporate N as a dopant. Nanowires with a controlled N concentration (atomic ratio of N to Zn) up to approximately 4% were prepared by varying the annealing time. X-ray photoelectron spectroscopy studies confirm N substitution at O sites in ZnO nanowires up to approximately 4%. Incident-photon-to-current-efficiency measurements carried out on PEC cell with ZnO:N nanowire arrays as photoanodes demonstrate a significant increase of photoresponse in the visible region compared to undoped ZnO nanowires prepared at similar conditions. Mott-Schottky measurements on a representative 3.7% ZnO:N sample give a flat-band potential of -0.58 V, a carrier density of approximately 4.6 x 10(18) cm(-3), and a space-charge layer of approximately 22 nm. Upon illumination at a power density of 100 mW/cm(2) (AM 1.5), water splitting is observed in both ZnO and ZnO:N nanowires. In comparison to ZnO nanowires without N-doping, ZnO:N nanowires show an order of magnitude increase in photocurrent density with photo-to-hydrogen conversion efficiency of 0.15% at an applied potential of +0.5 V (versus Ag/AgCl). These results suggest substantial potential of metal oxide nanowire arrays with controlled doping in PEC water splitting applications.
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              Solar hydrogen generation by a CdS-Au-TiO2 sandwich nanorod array enhanced with Au nanoparticle as electron relay and plasmonic photosensitizer.

              This paper presents a sandwich-structured CdS-Au-TiO2 nanorod array as the photoanode in a photoelectrochemical cell (PEC) for hydrogen generation via splitting water. The gold nanoparticles sandwiched between the TiO2 nanorod and the CdS quantum dot (QD) layer play a dual role in enhancing the solar-to-chemical energy conversion efficiency. First, the Au nanoparticles serve as an electron relay, which facilitates the charge transfer between CdS and TiO2 when the CdS QDs are photoexcited by wavelengths shorter than 525 nm. Second, the Au nanoparticles act as a plasmonic photosensitizer, which enables the solar-to-hydrogen conversion at wavelengths longer than the band edge of CdS, extending the photoconversion wavelength from 525 to 725 nm. The dual role of Au leads to a photocurrent of 4.07 mA/cm(2) at 0 V (vs Ag|AgCl) under full solar spectrum irradiation and a maximum solar-to-chemical energy conversion efficiency of 2.8%. An inversion analysis is applied to the transient absorption spectroscopy data, tracking the transfer of electrons and holes in the heterostructure, relating the relaxation dynamics to the underlying coupled rate equation and revealing that trap-state Auger recombination is a dominant factor in interfacial charge transfer. It is found that addition of Au nanoparticles increases the charge-transfer lifetime, reduces the trap-state Auger rate, suppresses the long-time scale back transfer, and partially compensates the negative effects of the surface trap states. Finally, the plasmonic energy-transfer mechanism is identified as direct transfer of the plasmonic hot carriers, and the interfacial Schottky barrier height is shown to modulate the plasmonic hot electron transfer and back transfer. Transient absorption characterization of the charge transfer shows defect states cannot be ignored when designing QD-sensitized solar cells. This facile sandwich structure combines both the electrical and the optical functions of Au nanoparticles into a single structure, which has implications for the design of efficient solar-energy-harvesting devices.
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                Author and article information

                Journal
                Sci Rep
                Sci Rep
                Scientific Reports
                Nature Publishing Group
                2045-2322
                02 June 2016
                2016
                : 6
                : 27241
                Affiliations
                [1 ]Key Laboratory for Organic Electronics and Information Displays & Institute of Advanced Materials (IAM), Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), Nanjing University of Posts & Telecommunications , Nanjing 210023, China
                [2 ]Key Laboratory of Flexible Electronics (KLOFE) & Institute of Advanced Materials (IAM), Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), Nanjing Tech University (NanjingTech) , Nanjing 211816, China
                Author notes
                Article
                srep27241
                10.1038/srep27241
                4890116
                27250648
                51152543-acc3-4672-adac-69be5e6a882e
                Copyright © 2016, Macmillan Publishers Limited

                This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/

                History
                : 12 April 2016
                : 16 May 2016
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