ZnO As an Active and Selective Catalyst for Electrochemical Water Oxidation to Hydrogen Peroxide
Abstract
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.
- Authors:
-
- 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:
- 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:
- 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.
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
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.
@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},
journal = {ACS Catalysis},
number = 5,
volume = 9,
place = {United States},
year = {Thu Apr 11 00:00:00 EDT 2019},
month = {Thu Apr 11 00:00:00 EDT 2019}
}
Web of Science
Works referenced in this record:
Global Hydrological Cycles and World Water Resources
journal, August 2006
- Oki, T.
- Science, Vol. 313, Issue 5790
Nonpoint Pollution of Surface Waters with Phosphorus and Nitrogen
journal, August 1998
- Carpenter, S. R.; Caraco, N. F.; Correll, D. L.
- Ecological Applications, Vol. 8, Issue 3
Direct Synthesis of Hydrogen Peroxide Over Au–Pd Catalysts Prepared by Electroless Deposition
journal, September 2015
- Alba-Rubio, Ana C.; Plauck, Anthony; Stangland, Eric E.
- Catalysis Letters, Vol. 145, Issue 12
Switching Off Hydrogen Peroxide Hydrogenation in the Direct Synthesis Process
journal, February 2009
- Edwards, J. K.; Solsona, B.; N., E. N.
- Science, Vol. 323, Issue 5917
Unifying the 2e – and 4e – Reduction of Oxygen on Metal Surfaces
journal, September 2012
- Viswanathan, Venkatasubramanian; Hansen, Heine Anton; Rossmeisl, Jan
- The Journal of Physical Chemistry Letters, Vol. 3, Issue 20
Enabling direct H2O2 production through rational electrocatalyst design
journal, November 2013
- Siahrostami, Samira; Verdaguer-Casadevall, Arnau; Karamad, Mohammadreza
- Nature Materials, Vol. 12, Issue 12
Trends in the Electrochemical Synthesis of H 2 O 2 : Enhancing Activity and Selectivity by Electrocatalytic Site Engineering
journal, February 2014
- Verdaguer-Casadevall, Arnau; Deiana, Davide; Karamad, Mohammadreza
- Nano Letters, Vol. 14, Issue 3
Designing Boron Nitride Islands in Carbon Materials for Efficient Electrochemical Synthesis of Hydrogen Peroxide
journal, May 2018
- Chen, Shucheng; Chen, Zhihua; Siahrostami, Samira
- Journal of the American Chemical Society, Vol. 140, Issue 25
Defective Carbon-Based Materials for the Electrochemical Synthesis of Hydrogen Peroxide
journal, November 2017
- Chen, Shucheng; Chen, Zhihua; Siahrostami, Samira
- ACS Sustainable Chemistry & Engineering, Vol. 6, Issue 1
Toward the Decentralized Electrochemical Production of H 2 O 2 : A Focus on the Catalysis
journal, March 2018
- Yang, Sungeun; Verdaguer-Casadevall, Arnau; Arnarson, Logi
- ACS Catalysis, Vol. 8, Issue 5
Toward the rational design of non-precious transition metal oxides for oxygen electrocatalysis
journal, January 2015
- Hong, Wesley T.; Risch, Marcel; Stoerzinger, Kelsey A.
- Energy & Environmental Science, Vol. 8, Issue 5
An Investigation of Thin-Film Ni–Fe Oxide Catalysts for the Electrochemical Evolution of Oxygen
journal, August 2013
- Louie, Mary W.; Bell, Alexis T.
- Journal of the American Chemical Society, Vol. 135, Issue 33
Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces
journal, March 2011
- Man, Isabela C.; Su, Hai‐Yan; Calle‐Vallejo, Federico
- ChemCatChem, Vol. 3, Issue 7
Homogeneously dispersed multimetal oxygen-evolving catalysts
journal, March 2016
- Zhang, B.; Zheng, X.; Voznyy, O.
- Science, Vol. 352, Issue 6283
Electrochemical Water Oxidation with Cobalt-Based Electrocatalysts from pH 0–14: The Thermodynamic Basis for Catalyst Structure, Stability, and Activity
journal, August 2011
- Gerken, James B.; McAlpin, J. Gregory; Chen, Jamie Y. C.
- Journal of the American Chemical Society, Vol. 133, Issue 36
Selective Electrochemical Generation of Hydrogen Peroxide from Water Oxidation
journal, October 2015
- Viswanathan, Venkatasubramanian; Hansen, Heine A.; Nørskov, Jens K.
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 21
Enhanced Oxidative Hydrogen Peroxide Production on Conducting Glass Anodes Modified with Metal Oxides
journal, November 2016
- Fuku, Kojiro; Miyase, Yuta; Miseki, Yugo
- ChemistrySelect, Vol. 1, Issue 18
Understanding activity trends in electrochemical water oxidation to form hydrogen peroxide
journal, September 2017
- Shi, Xinjian; Siahrostami, Samira; Li, Guo-Ling
- Nature Communications, Vol. 8, Issue 1
CaSnO 3 : An Electrocatalyst for Two-Electron Water Oxidation Reaction to Form H 2 O 2
journal, December 2018
- Park, So Yeon; Abroshan, Hadi; Shi, Xinjian
- ACS Energy Letters, Vol. 4, Issue 1
One- or Two-Electron Water Oxidation, Hydroxyl Radical, or H 2 O 2 Evolution
journal, February 2017
- Siahrostami, Samira; Li, Guo-Ling; Viswanathan, Venkatasubramanian
- The Journal of Physical Chemistry Letters, Vol. 8, Issue 6
Photochemical Synthesis of Hydrogen Peroxide at Zinc Oxide Surfaces 1
journal, June 1953
- Rubin, Thor R.; Calvert, Jack G.; Rankin, George T.
- Journal of the American Chemical Society, Vol. 75, Issue 12
H2O2 Formation from photocatalytic processes at the ZnO/water interface
journal, July 2001
- Domènech, Xavier; Ayllón, José Antonio; Peral, José
- Environmental Science and Pollution Research, Vol. 8, Issue 4
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Improved adsorption energetics within density-functional theory using revised Perdew-Burke-Ernzerhof functionals
journal, March 1999
- Hammer, B.; Hansen, L. B.; Nørskov, J. K.
- Physical Review B, Vol. 59, Issue 11
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
A Linear Response DFT+ U Study of Trends in the Oxygen Evolution Activity of Transition Metal Rutile Dioxides
journal, February 2015
- Xu, Zhongnan; Rossmeisl, Jan; Kitchin, John R.
- The Journal of Physical Chemistry C, Vol. 119, Issue 9
Thermochemistry and micro-kinetic analysis of methanol synthesis on ZnO (0001)
journal, January 2014
- Medford, Andrew J.; Sehested, Jens; Rossmeisl, Jan
- Journal of Catalysis, Vol. 309
Ferromagnetic behavior of high-purity ZnO nanoparticles
journal, January 2011
- Escudero, R.; Escamilla, R.
- Solid State Communications, Vol. 151, Issue 2
The chemistry and physics of zinc oxide surfaces
journal, January 2007
- Woll, C.
- Progress in Surface Science, Vol. 82, Issue 2-3
Competing stabilization mechanism for the polar ZnO(0001)-Zn surface
journal, December 2003
- Kresse, Georg; Dulub, Olga; Diebold, Ulrike
- Physical Review B, Vol. 68, Issue 24
Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode
journal, November 2004
- Nørskov, J. K.; Rossmeisl, J.; Logadottir, A.
- The Journal of Physical Chemistry B, Vol. 108, Issue 46
Implicit solvation model for density-functional study of nanocrystal surfaces and reaction pathways
journal, February 2014
- Mathew, Kiran; Sundararaman, Ravishankar; Letchworth-Weaver, Kendra
- The Journal of Chemical Physics, Vol. 140, Issue 8
Influence of Adsorbed Water on the Oxygen Evolution Reaction on Oxides
journal, December 2014
- Siahrostami, S.; Vojvodic, A.
- The Journal of Physical Chemistry C, Vol. 119, Issue 2
Solvation Effects for Oxygen Evolution Reaction Catalysis on IrO 2 (110)
journal, May 2017
- Gauthier, Joseph A.; Dickens, Colin F.; Chen, Leanne D.
- The Journal of Physical Chemistry C, Vol. 121, Issue 21
O 2 Reduction Mechanism on Non-Noble Metal Catalysts for PEM Fuel Cells. Part I: Experimental Rates of O 2 Electroreduction, H 2 O 2 Electroreduction, and H 2 O 2 Disproportionation
journal, July 2009
- Jaouen, Frédéric; Dodelet, Jean-Pol
- The Journal of Physical Chemistry C, Vol. 113, Issue 34
Tailoring the Activity for Oxygen Evolution Electrocatalysis on Rutile TiO2(110) by Transition-Metal Substitution
journal, August 2011
- García-Mota, Mónica; Vojvodic, Aleksandra; Metiu, Horia
- ChemCatChem, Vol. 3, Issue 10
Effects of Anions and pH on the Stability of ZnO Nanorods for Photoelectrochemical Water Splitting
journal, March 2018
- Liu, Ching-Fang; Lu, Yi-Jing; Hu, Chi-Chang
- ACS Omega, Vol. 3, Issue 3
Works referencing / citing this record:
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
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
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