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Title: Selective and Efficient Gd-Doped BiVO4 Photoanode for Two-Electron Water Oxidation to H2O2

Abstract

Photoelectrochemical oxidation of water presents a pathway for sustainable production of hydrogen peroxide (H2O2). Here two-electron water oxidation toward H2O2, however, competes with the popular four-electron process to form oxygen and one-electron water oxidation to form OH radical. To date, bismuth vanadate (BiVO4) has been shown to exhibit promising selectivity toward H2O2, especially under illumination, but it suffers from high overpotential and notoriously poor stability. Herein, using density functional theory calculations, we predict that doping BiVO4 with optimal concentrations of gadolinium (Gd) not only enhances its activity for H2O2 production but also improves its stability. Experimentally, we demonstrate that intermediate amounts of Gd doping (6–12%) reduce the onset potential of BiVO4 for H2O2 production by ~110 mV while achieving a Faradaic efficiency of ~99.5% under illumination and prolonging the catalytic lifetime by more than a factor of 20 at 2.0 V vs RHE under illumination.

Authors:
 [1];  [2]; ORCiD logo [2];  [2];  [2];  [3]; ORCiD logo [4]; ORCiD logo [2]; ORCiD logo [2]
  1. Stanford Univ., Stanford, CA (United States); Sungkyunkwan Univ., Suwon (Republic of Korea)
  2. Stanford Univ., Stanford, CA (United States)
  3. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Sungkyunkwan Univ., Suwon (Republic of Korea)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1505428
Grant/Contract Number:  
AC02-76SF00515; 2012M3A6A7054855; 2016M3D1A1027664; 2017R1A2B3010927
Resource Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 4; Journal Issue: 3; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Baek, Ji Hyun, Gill, Thomas Mark, Abroshan, Hadi, Park, Sangwook, Shi, Xinjian, Nørskov, Jens, Jung, Hyun Suk, Siahrostami, Samira, and Zheng, Xiaolin. Selective and Efficient Gd-Doped BiVO4 Photoanode for Two-Electron Water Oxidation to H2O2. United States: N. p., 2019. Web. doi:10.1021/acsenergylett.9b00277.
Baek, Ji Hyun, Gill, Thomas Mark, Abroshan, Hadi, Park, Sangwook, Shi, Xinjian, Nørskov, Jens, Jung, Hyun Suk, Siahrostami, Samira, & Zheng, Xiaolin. Selective and Efficient Gd-Doped BiVO4 Photoanode for Two-Electron Water Oxidation to H2O2. United States. https://doi.org/10.1021/acsenergylett.9b00277
Baek, Ji Hyun, Gill, Thomas Mark, Abroshan, Hadi, Park, Sangwook, Shi, Xinjian, Nørskov, Jens, Jung, Hyun Suk, Siahrostami, Samira, and Zheng, Xiaolin. Fri . "Selective and Efficient Gd-Doped BiVO4 Photoanode for Two-Electron Water Oxidation to H2O2". United States. https://doi.org/10.1021/acsenergylett.9b00277. https://www.osti.gov/servlets/purl/1505428.
@article{osti_1505428,
title = {Selective and Efficient Gd-Doped BiVO4 Photoanode for Two-Electron Water Oxidation to H2O2},
author = {Baek, Ji Hyun and Gill, Thomas Mark and Abroshan, Hadi and Park, Sangwook and Shi, Xinjian and Nørskov, Jens and Jung, Hyun Suk and Siahrostami, Samira and Zheng, Xiaolin},
abstractNote = {Photoelectrochemical oxidation of water presents a pathway for sustainable production of hydrogen peroxide (H2O2). Here two-electron water oxidation toward H2O2, however, competes with the popular four-electron process to form oxygen and one-electron water oxidation to form OH radical. To date, bismuth vanadate (BiVO4) has been shown to exhibit promising selectivity toward H2O2, especially under illumination, but it suffers from high overpotential and notoriously poor stability. Herein, using density functional theory calculations, we predict that doping BiVO4 with optimal concentrations of gadolinium (Gd) not only enhances its activity for H2O2 production but also improves its stability. Experimentally, we demonstrate that intermediate amounts of Gd doping (6–12%) reduce the onset potential of BiVO4 for H2O2 production by ~110 mV while achieving a Faradaic efficiency of ~99.5% under illumination and prolonging the catalytic lifetime by more than a factor of 20 at 2.0 V vs RHE under illumination.},
doi = {10.1021/acsenergylett.9b00277},
journal = {ACS Energy Letters},
number = 3,
volume = 4,
place = {United States},
year = {2019},
month = {2}
}

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