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Title: A photochemical diode artificial photosynthesis system for unassisted high efficiency overall pure water splitting

Abstract

The conversion of solar energy into chemical fuels can potentially address many of the energy and environment related challenges we face today. In this study, we have demonstrated a photochemical diode artificial photosynthesis system that can enable efficient, unassisted overall pure water splitting without using any sacrificial reagent. By precisely controlling charge carrier flow at the nanoscale, the wafer-level photochemical diode arrays exhibited solar-to-hydrogen efficiency ~3.3% in neutral (pH ~ 7.0) overall water splitting reaction. In part of the visible spectrum (400–485 nm), the energy conversion efficiency and apparent quantum yield reaches ~8.75% and ~20%, respectively, which are the highest values ever reported for one-step visible-light driven photocatalytic overall pure water splitting. The effective manipulation and control of charge carrier flow in nanostructured photocatalysts provides critical insight in achieving high efficiency artificial photosynthesis, including the efficient and selective reduction of CO 2 to hydrocarbon fuels.

Authors:
 [1];  [2];  [1];  [3]
  1. McGill Univ., Montreal, QC (Canada)
  2. Center of Excellence in Transportation Electrification and Energy Storage (CETEES), Varennes, QC (United States)
  3. Univ. of Michigan, Ann Arbor, MI (United States); McGill Univ., Montreal, QC (Canada)
Publication Date:
Research Org.:
Univ. of Michigan, Ann Arbor, MI (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Fuel Cell Technologies Office (EE-3F)
OSTI Identifier:
1500016
Grant/Contract Number:  
EE0008086
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING

Citation Formats

Chowdhury, Faqrul A., Trudeau, Michel L., Guo, Hong, and Mi, Zetian. A photochemical diode artificial photosynthesis system for unassisted high efficiency overall pure water splitting. United States: N. p., 2018. Web. doi:10.1038/s41467-018-04067-1.
Chowdhury, Faqrul A., Trudeau, Michel L., Guo, Hong, & Mi, Zetian. A photochemical diode artificial photosynthesis system for unassisted high efficiency overall pure water splitting. United States. doi:10.1038/s41467-018-04067-1.
Chowdhury, Faqrul A., Trudeau, Michel L., Guo, Hong, and Mi, Zetian. Fri . "A photochemical diode artificial photosynthesis system for unassisted high efficiency overall pure water splitting". United States. doi:10.1038/s41467-018-04067-1. https://www.osti.gov/servlets/purl/1500016.
@article{osti_1500016,
title = {A photochemical diode artificial photosynthesis system for unassisted high efficiency overall pure water splitting},
author = {Chowdhury, Faqrul A. and Trudeau, Michel L. and Guo, Hong and Mi, Zetian},
abstractNote = {The conversion of solar energy into chemical fuels can potentially address many of the energy and environment related challenges we face today. In this study, we have demonstrated a photochemical diode artificial photosynthesis system that can enable efficient, unassisted overall pure water splitting without using any sacrificial reagent. By precisely controlling charge carrier flow at the nanoscale, the wafer-level photochemical diode arrays exhibited solar-to-hydrogen efficiency ~3.3% in neutral (pH ~ 7.0) overall water splitting reaction. In part of the visible spectrum (400–485 nm), the energy conversion efficiency and apparent quantum yield reaches ~8.75% and ~20%, respectively, which are the highest values ever reported for one-step visible-light driven photocatalytic overall pure water splitting. The effective manipulation and control of charge carrier flow in nanostructured photocatalysts provides critical insight in achieving high efficiency artificial photosynthesis, including the efficient and selective reduction of CO2 to hydrocarbon fuels.},
doi = {10.1038/s41467-018-04067-1},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {4}
}

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Cited by: 34 works
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Figures / Tables:

Fig. 1 Fig. 1 : Structural and optical properties of InGaN photochemical diode. a Schematic illustration of wafer-level unassisted photocatalytic overall water splitting on double-band nanowire arrays36, which are vertically aligned on a planar substrate and decorated with co-catalysts for hydrogen evolution reaction (HER). Unlike tandem PEC cells or photovoltaic (PV) devices66–69more » this approach does not require any carrier recombination/transfer or current matching between the layers along vertical direction. Both water oxidation and proton reduction reaction occur on the radial non-polar surfaces of each layer. b Energy-band representation of the proposed photochemical diode (PCD) with radial thicknes “d” showing the built-in electric field (band-bending) that separates the charge carriers (electron and hole) and drives towards the opposite cathode and anode surfaces. In contrast to conventional p-n PCD (Supplementary Fig. 1 and Supplementary Note 1), only single photon absorption is required to generate one active electron–hole pair to participate in redox reaction (like Schottky-type photochemical diode). c A 45° tilted SEM image of InGaN:Mg PCD nanostructures, vertically aligned on Si substrate. Scale bar, 1 µm. The magnified image of the nanosheets is also presented in the inset for clarity. d Schematic (real space) depiction of the dynamic behaviors of charge carriers in a single-photon PCD upon photoexcitation. Electron enriched surface (cathode) of the PCD is largely decorated with photo-deposited HER co-catalysts (Rh/Cr2O3 core/shell nanoparticles). e Room temperature photoluminescence (PL) spectrum from as-grown p-InGaN PCDs for different indium incorporations (correspond to different bandgaps, depicted using distinct colors). The inset shows ~20-fold reduction in PL intensity for the photochemical diodes compared to that of nanowires« less

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      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.