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Nano-Photoelectrochemical Cell Arrays with Spatially Isolated Oxidation and Reduction Channels

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Department of Materials Science and Engineering, Carnegie Mellon University, 5000 Forbes Avenue, Pittsburgh, Pennsylvania 15213-3890, United States
Cite this: ACS Nano 2017, 11, 2, 2150–2159
Publication Date (Web):January 17, 2017
Copyright © 2017 American Chemical Society

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    Photoelectrochemical conversion of solar energy is explored for many diverse applications but suffers from poor efficiencies due to limited solar absorption, inadequate charge carrier separation, redox half-reactions occurring in close proximity, and/or long ion diffusion lengths. We have taken a drastically different approach to the design of photoelectrochemical cells (PECs) to spatially isolate reaction sites at the nanoscale to different materials and flow channels, suppressing carrier recombination and back-reaction of intermediates while shortening ion diffusion paths and, importantly, avoiding mixed product generation. We developed massively parallel nano-PECs composed of an array of open-ended carbon nanotubes (CNTs) with photoanodic reactions occurring on the outer walls, uniformly coated with titanium dioxide (TiO2), and photocathodic reactions occurring on the inner walls, decorated with platinum (Pt). We verified the redox reaction isolation by demonstrating selective photodeposition of manganese oxide on the outside and silver on the inside of the TiO2/CNT/Pt nanotubes. Further, the nano-PECs exhibit improved solar absorption and efficient charge transfer of photogenerated carriers to their respective redox sites, leading to a 1.8% photon-to-current conversion efficiency (a current density of 4.2 mA/cm2) under white-light irradiation. The design principles demonstrated can be readily adapted to myriads of photocatalysts for cost-effective solar utilization.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsnano.6b08387.

    • Figures of (1) TGA of TiO2/CNT membrane, (2) high-resolution TEM image of TiO2/CNT/Pt membranes, (3) adsorption isotherms and pore characteristics of TiO2/CNT membranes, (4) adsorption–desorption equilibration time of methylene blue dye on TiO2/CNT/Pt and TiO2/CNT membranes in the dark, (5) dye absorption spectra at various reaction time intervals, (6) photocatalytic methylene blue dye degradation of TiO2/CNT and TiO2/CNT/Pt membrane under white-light, (7) SEM image of TiO2/CNT/Pt membrane after being filled with PVA polymer, (8) J–V curves of TiO2/CNT/Pt membrane on the RHE scale, (9) ΔJ–V curves on an RHE scale for TiO2/CNT membranes under white- and visible-light, (10) ΔJ–V curves on an RHE scale by TiO2, TiO2/Pt, CNT, CNT/Pt membranes under white- and visible-light, (11) TEM images of MnOx flakes on the outer wall surface and Ag nanoparticles on the inside of TiO2/CNT/Pt nanotubes, and (12) conventional-resolution TEM images of photodeposited Ag nanoparticles on the interior CNT wall of TiO2/CNT/Pt membranes (PDF)

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