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General Layer-by-Layer Assembly of Multilayered Photoanodes: Triggering Tandem Charge Transport toward Photoelectrochemical Water Oxidation

  • Shuo Hou
    Shuo Hou
    College of Materials Science and Engineering, Fuzhou University, New Campus, Minhou, Fujian Province 350108, China
    More by Shuo Hou
  • Zhi-Quan Wei
    Zhi-Quan Wei
    College of Materials Science and Engineering, Fuzhou University, New Campus, Minhou, Fujian Province 350108, China
    More by Zhi-Quan Wei
  • Xiao-Cheng Dai
    Xiao-Cheng Dai
    College of Materials Science and Engineering, Fuzhou University, New Campus, Minhou, Fujian Province 350108, China
  • Ming-Hui Huang
    Ming-Hui Huang
    College of Materials Science and Engineering, Fuzhou University, New Campus, Minhou, Fujian Province 350108, China
  • , and 
  • Fang-Xing Xiao*
    Fang-Xing Xiao
    College of Materials Science and Engineering, Fuzhou University, New Campus, Minhou, Fujian Province 350108, China
    *E-mail: [email protected]
Cite this: Inorg. Chem. 2020, 59, 10, 7325–7334
Publication Date (Web):April 27, 2020
https://doi.org/10.1021/acs.inorgchem.0c00780
Copyright © 2020 American Chemical Society
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Abstract

Modulation of photoinduced charge separation/migration and construction of controllable charge transfer pathway over photoelectrodes have been attracting enduring interest in semiconductor-based photoelectrochemical (PEC) cells but suffer from sluggish charge transport kinetics. Here, we report a general approach to fabricate NP-TNTAs/(TMCs QDs/PSS)n (X = Te, Se, S) photoanodes via a facile and green electrostatic layer-by-layer (LbL) self-assembly strategy, for which transition-metal chalcogenides quantum dots (TMCs QDs) [CdX (X = Se, Te, S)] and poly(sodium 4-styrenesulfonate) (PSS) were periodically deposited on the nanoporous TiO2 nanotube arrays (NP-TNTAs) via substantial electrostatic force, resulting in the continuous charge transfer pathway. NP-TNTAs/(TMCs QDs/PSS)n photoanodes demonstrate significantly enhanced solar-driven photoelectrochemical (PEC) water oxidation activities, relative to NP-TNTAs and TMCs QDs under visible and simulated sunlight irradiation, predominantly because of the suitable energy level configuration between NP-TNTAs and TMCs QDs, unique integration mode, and high-speed interfacial charge separation rate endowed by LbL assembly. The ultrathin PSS intermediate layer functions as “molecule glue” for pinpoint and uniform self-assembly of TMCs QDs on the framework of NP-TNTAs and photosensitization effect of TMCs QDs triggers the unidirectional charge transfer cascade, synergistically boosting the charge separation/transfer efficiency. Our work offers an efficacious approach to craft multilayered photoelectrodes and spur further interest in finely tuning the spatial charge flow in PEC cell for solar-to-hydrogen conversion.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.inorgchem.0c00780.

  • Experimental section describing the materials, preparation of NP-TNTAs, preparation of positively charged CdTe, CdSe, CdS QDs, and PEC water splitting measurements; supplemental figures (S1−S18) and tables (S1 and S2) (PDF)

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