ZnO As an Active and Selective Catalyst for Electrochemical Water Oxidation to Hydrogen Peroxide

doi:https://doi.org/10.1021/acscatal.8b04873

Title: ZnO As an Active and Selective Catalyst for Electrochemical Water Oxidation to Hydrogen Peroxide

Abstract

Electrochemical synthesis of hydrogen peroxide (H ₂O ₂) via two-electron water oxidation reaction (2e-WOR) is an ideal process for delocalized production for water cleaning and other applications. Previously observed water oxidation catalysts have limited activity and selectivity, imposing a bottleneck for broad adoption of this technology. We determine ZnO as a new stable, nontoxic, active, and selective catalyst for 2e-WOR to generate H ₂O ₂. Using density functional theory calculations, we propose that the (1010) facet of ZnO is an effective catalyst for 2e-WOR and confirm the prediction experimentally. We synthesize ZnO nanoparticles with a high fraction of (1010) facets and find that this catalyst gives an overpotential of 40 mV at 0.1 mA/cm ² and peak Faradaic efficiency of 81% toward H ₂O ₂ evolution.

Authors:

^[1]; Shi, Xinjian ^[1];

^[1]; Vallez, Lauren ^[1];

^[2];

^[3];

^[1]; Nørskov, Jens K. ^[4]

Stanford Univ., CA (United States)
Stanford Univ., CA (United States); Sungkyunkwan Univ., Suwon (Republic of Korea)
Stanford Univ., CA (United States); Univ. of Calgary, AB (Canada)
Stanford Univ., CA (United States) ; SLAC National Accelerator Lab., Menlo Park, CA (United States); Technical Univ. of Denmark, Lyngby (Denmark)

Publication Date:: 2019-04-11

Research Org.:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1529320

Grant/Contract Number:: AC02-76SF00515; SC0008685

Resource Type:: Journal Article: Accepted Manuscript

Journal Name:: ACS Catalysis

Additional Journal Information:: Journal Volume: 9; Journal Issue: 5; Journal ID: ISSN 2155-5435

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; water oxidation catalysis; hydrogen peroxide synthesis; zinc oxide; density functional theory; electrocatalysis

Citation Formats


                    Kelly, Sara R., Shi, Xinjian, Back, Seoin, Vallez, Lauren, Park, So Yeon, Siahrostami, Samira, Zheng, Xiaolin, and Nørskov, Jens K. ZnO As an Active and Selective Catalyst for Electrochemical Water Oxidation to Hydrogen Peroxide.  United States: N. p., 2019. 
        Web.  doi:10.1021/acscatal.8b04873.

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                    Kelly, Sara R., Shi, Xinjian, Back, Seoin, Vallez, Lauren, Park, So Yeon, Siahrostami, Samira, Zheng, Xiaolin, & Nørskov, Jens K. ZnO As an Active and Selective Catalyst for Electrochemical Water Oxidation to Hydrogen Peroxide.  United States.  https://doi.org/10.1021/acscatal.8b04873

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                    Kelly, Sara R., Shi, Xinjian, Back, Seoin, Vallez, Lauren, Park, So Yeon, Siahrostami, Samira, Zheng, Xiaolin, and Nørskov, Jens K. Thu .  
        "ZnO As an Active and Selective Catalyst for Electrochemical Water Oxidation to Hydrogen Peroxide".  United States.  https://doi.org/10.1021/acscatal.8b04873.  https://www.osti.gov/servlets/purl/1529320.

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@article{osti_1529320,

  title        = {ZnO As an Active and Selective Catalyst for Electrochemical Water Oxidation to Hydrogen Peroxide},

  author       = {Kelly, Sara R. and Shi, Xinjian and Back, Seoin and Vallez, Lauren and Park, So Yeon and Siahrostami, Samira and Zheng, Xiaolin and Nørskov, Jens K.},

  abstractNote = {Electrochemical synthesis of hydrogen peroxide (H2O2) via two-electron water oxidation reaction (2e-WOR) is an ideal process for delocalized production for water cleaning and other applications. Previously observed water oxidation catalysts have limited activity and selectivity, imposing a bottleneck for broad adoption of this technology. We determine ZnO as a new stable, nontoxic, active, and selective catalyst for 2e-WOR to generate H2O2. Using density functional theory calculations, we propose that the (1010) facet of ZnO is an effective catalyst for 2e-WOR and confirm the prediction experimentally. We synthesize ZnO nanoparticles with a high fraction of (1010) facets and find that this catalyst gives an overpotential of 40 mV at 0.1 mA/cm2 and peak Faradaic efficiency of 81% toward H2O2 evolution.},

  doi          = {10.1021/acscatal.8b04873},

  url          = {https://www.osti.gov/biblio/1529320},
  journal      = {ACS Catalysis},

  issn         = {2155-5435},

  number       = 5,

  volume       = 9,

  place        = {United States},

  year         = {2019},

  month        = {4}

}

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Journal Article:

Free Publicly Available Full Text

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https://doi.org/10.1021/acscatal.8b04873

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Cited by: 11 works

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Works referencing / citing this record:

Confined local oxygen gas promotes electrochemical water oxidation to hydrogen peroxide
journal, January 2020

Xia, Chuan; Back, Seoin; Ringe, Stefan
Nature Catalysis, Vol. 3, Issue 2
https://doi.org/10.1038/s41929-019-0402-8

Hydrogen peroxide electrochemical synthesis on hybrid double-atom (Pd–Cu) doped N vacancy g-C ₃ N ₄ : a novel design strategy for electrocatalyst screening
journal, January 2020

Cao, Yongyong; Zhao, Chenxia; Fang, Qiaojun
Journal of Materials Chemistry A, Vol. 8, Issue 5
https://doi.org/10.1039/c9ta12468c

Electrochemical H ₂ O ₂ Production and Accumulation from H ₂ O by Composite Effect of Al ₂ O ₃ and BiVO ₄
journal, January 2019

Miyase, Yuta; Iguchi, Shoji; Miseki, Yugo
Journal of The Electrochemical Society, Vol. 166, Issue 13
https://doi.org/10.1149/2.0561913jes

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Title: ZnO As an Active and Selective Catalyst for Electrochemical Water Oxidation to Hydrogen Peroxide

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Citation Formats

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