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Title: Highly Enhanced Photoelectrochemical Water Oxidation Efficiency Based on Triadic Quantum Dot/Layered Double Hydroxide/BiVO 4 Photoanodes

The water oxidation half-reaction is considered to be a bottleneck for achieving highly efficient solar-driven water splitting due to its multiproton-coupled four-electron process and sluggish kinetics. Herein, a triadic photoanode consisting of dual-sized CdTe quantum dots (QDs), Co-based layered double hydroxide (LDH) nanosheets, and BiVO4 particles, that is, QD@LDH@BiVO4, was designed. Two sets of consecutive Type-II band alignments were constructed to improve photogenerated electron-hole separation in the triadic structure. The efficient charge separation resulted in a 2-fold enhancement of the photocurrent of the QD@LDH@BiVO4 photoanode. A significantly enhanced oxidation efficiency reaching above 90% in the low bias region (i.e., E < 0.8 V vs RHE) could be critical in determining the overall performance of a complete photoelectrochemical cell. The faradaic efficiency for water oxidation was almost 90%. The conduction band energy of QDs is -1.0 V more negative than that of LDH, favorable for the electron injection to LDH and enabling a more efficient hole separation. The enhanced photon-to-current conversion efficiency and improved water oxidation efficiency of the triadic structure may result from the non-negligible contribution of hot electrons or holes generated in QDs. Such a band-matching and multidimensional triadic architecture could be a promising strategy for achieving high-efficiency photoanodesmore » by sufficiently utilizing and maximizing the functionalities of QDs.« less
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Publication Date:
OSTI Identifier:
Report Number(s):
Journal ID: ISSN 1944-8244
DOE Contract Number:
Resource Type:
Journal Article
Resource Relation:
Journal Name: ACS Applied Materials and Interfaces; Journal Volume: 8; Journal Issue: 30
American Chemical Society
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Country of Publication:
United States
36 MATERIALS SCIENCE; layered double hydroxides; photoanodes; photoelectrochemistry; quantum dots; water oxidation