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Title: Electrochemical Reduction Properties of Extended Space Charge InGaP and GaP Epitaxial Layers

Abstract

Two lattice-matched epitaxial III-V phosphide films of thicknesses between 400 and 500 nm are grown by metal-organic chemical vapor deposition: InGaP on GaAs and GaP on Si. These structures are designed as photocathodes for solar-driven chemical reduction processes such as the hydrogen evolution reaction (HER) and CO2 reduction into higher-order hydrocarbons. By using p+ substrates and undoped epitaxial layers, an extended space-charge active region is achieved in the electrode with a design analogous to a p-i-n solar cell. When in contact with the methyl viologen MV+ / + + redox couple, the InGaP/GaAs and GaP/Si cathodes generate a photovoltage of 388 mV and 274 mV, respectively, under 1 sun illumination. Incident photon-to-current efficiency (IPCE) measurements confirm that the undoped active layers are exclusively performing light absorption and minority carrier diffusion-based charge transfer of high-energy photons. This shows that performance can be significantly boosted with lower-doped substrates. The InGaP/GaAs and GaP/Si electrodes are shown to drive the HER at saturation photocurrent densities of 9.05 mA/cm2 and 2.34 mA/cm2, respectively, under 1 sun illumination without a co-catalyst and under a large reduction bias. As a result, thicker films did not show a corresponding increased performance, and can be explained through understanding ofmore » crystalline defects and the electrostatics of the junctions.« less

Authors:
 [1];  [1];  [1]
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  1. Stanford Univ., Stanford, CA (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center on Nanostructuring for Efficient Energy Conversion (CNEEC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1370006
Grant/Contract Number:  
SC0001060
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 163; Journal Issue: 8; Related Information: CNEEC partners with Stanford University (lead); Carnegie Institution at Stanford; Technical University of Denmark; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Parameshwaran, Vijay, Xu, Xiaoqing, and Clemens, Bruce. Electrochemical Reduction Properties of Extended Space Charge InGaP and GaP Epitaxial Layers. United States: N. p., 2016. Web. doi:10.1149/2.1341608jes.
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Parameshwaran, Vijay, Xu, Xiaoqing, & Clemens, Bruce. Electrochemical Reduction Properties of Extended Space Charge InGaP and GaP Epitaxial Layers. United States. https://doi.org/10.1149/2.1341608jes
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Parameshwaran, Vijay, Xu, Xiaoqing, and Clemens, Bruce. Fri . "Electrochemical Reduction Properties of Extended Space Charge InGaP and GaP Epitaxial Layers". United States. https://doi.org/10.1149/2.1341608jes. https://www.osti.gov/servlets/purl/1370006.
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@article{osti_1370006,
title = {Electrochemical Reduction Properties of Extended Space Charge InGaP and GaP Epitaxial Layers},
author = {Parameshwaran, Vijay and Xu, Xiaoqing and Clemens, Bruce},
abstractNote = {Two lattice-matched epitaxial III-V phosphide films of thicknesses between 400 and 500 nm are grown by metal-organic chemical vapor deposition: InGaP on GaAs and GaP on Si. These structures are designed as photocathodes for solar-driven chemical reduction processes such as the hydrogen evolution reaction (HER) and CO2 reduction into higher-order hydrocarbons. By using p+ substrates and undoped epitaxial layers, an extended space-charge active region is achieved in the electrode with a design analogous to a p-i-n solar cell. When in contact with the methyl viologen MV+ / + + redox couple, the InGaP/GaAs and GaP/Si cathodes generate a photovoltage of 388 mV and 274 mV, respectively, under 1 sun illumination. Incident photon-to-current efficiency (IPCE) measurements confirm that the undoped active layers are exclusively performing light absorption and minority carrier diffusion-based charge transfer of high-energy photons. This shows that performance can be significantly boosted with lower-doped substrates. The InGaP/GaAs and GaP/Si electrodes are shown to drive the HER at saturation photocurrent densities of 9.05 mA/cm2 and 2.34 mA/cm2, respectively, under 1 sun illumination without a co-catalyst and under a large reduction bias. As a result, thicker films did not show a corresponding increased performance, and can be explained through understanding of crystalline defects and the electrostatics of the junctions.},
doi = {10.1149/2.1341608jes},
journal = {Journal of the Electrochemical Society},
number = 8,
volume = 163,
place = {United States},
year = {Fri Jun 17 00:00:00 EDT 2016},
month = {Fri Jun 17 00:00:00 EDT 2016}
}
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Journal Article:
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https://doi.org/10.1149/2.1341608jes
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Figures / Tables:

Figure 1 Figure 1: (a) Band diagram of a p-type semiconductor in contact with a redox couple A/A−. (b) Proposed band diagram of a p+ semiconductor, with an intrinsic thin epitaxial layer, in contact with a redox couple A/A−. The intrinsic thin layer creates a space charge region that can effectively absorbmore » photons and extract electron-hole pairs. The redox couple A/A−, for reduction studies, is MV++/+ for non-aqueous experiments and H+/H2 for aqueous experiments.« less
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