DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: One- or two-electron water oxidation, hydroxyl radical, or H2O2 evolution

Abstract

Electrochemical or photoelectrochemcial oxidation of water to form hydrogen peroxide (H2O2) or hydroxyl radicals (•OH) offers a very attractive route to water disinfection, and the first process could be the basis for a clean way to produce hydrogen peroxide. A major obstacle in the development of effective catalysts for these reactions is that the electrocatalyst must suppress the thermodynamically favored four-electron pathway leading to O2 evolution. Here, we develop a thermochemical picture of the catalyst properties that determine selectivity toward the one, two, and four electron processes leading to •OH, H2O2, and O2.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3];  [4]
  1. Stanford Univ., Stanford, CA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States); Henan Univ. of Science and Technology, Luoyang (China)
  3. Carnegie Mellon Univ., Pittsburgh, PA (United States)
  4. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
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:
1350735
Grant/Contract Number:  
52454; AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 8; Journal Issue: 6; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Siahrostami, Samira, Li, Guo -Ling, Viswanathan, Venkatasubramanian, and Nørskov, Jens K. One- or two-electron water oxidation, hydroxyl radical, or H2O2 evolution. United States: N. p., 2017. Web. doi:10.1021/acs.jpclett.6b02924.
Siahrostami, Samira, Li, Guo -Ling, Viswanathan, Venkatasubramanian, & Nørskov, Jens K. One- or two-electron water oxidation, hydroxyl radical, or H2O2 evolution. United States. https://doi.org/10.1021/acs.jpclett.6b02924
Siahrostami, Samira, Li, Guo -Ling, Viswanathan, Venkatasubramanian, and Nørskov, Jens K. Thu . "One- or two-electron water oxidation, hydroxyl radical, or H2O2 evolution". United States. https://doi.org/10.1021/acs.jpclett.6b02924. https://www.osti.gov/servlets/purl/1350735.
@article{osti_1350735,
title = {One- or two-electron water oxidation, hydroxyl radical, or H2O2 evolution},
author = {Siahrostami, Samira and Li, Guo -Ling and Viswanathan, Venkatasubramanian and Nørskov, Jens K.},
abstractNote = {Electrochemical or photoelectrochemcial oxidation of water to form hydrogen peroxide (H2O2) or hydroxyl radicals (•OH) offers a very attractive route to water disinfection, and the first process could be the basis for a clean way to produce hydrogen peroxide. A major obstacle in the development of effective catalysts for these reactions is that the electrocatalyst must suppress the thermodynamically favored four-electron pathway leading to O2 evolution. Here, we develop a thermochemical picture of the catalyst properties that determine selectivity toward the one, two, and four electron processes leading to •OH, H2O2, and O2.},
doi = {10.1021/acs.jpclett.6b02924},
journal = {Journal of Physical Chemistry Letters},
number = 6,
volume = 8,
place = {United States},
year = {Thu Feb 23 00:00:00 EST 2017},
month = {Thu Feb 23 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 161 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Standard electrode potentials involving radicals in aqueous solution: inorganic radicals
journal, January 2013

  • Armstrong, David A.; Huie, Robert E.; Lymar, Sergei
  • BioInorganic Reaction Mechanisms, Vol. 9, Issue 1-4
  • DOI: 10.1515/irm-2013-0005

Hydrogen Peroxide Synthesis: An Outlook beyond the Anthraquinone Process
journal, October 2006

  • Campos-Martin, Jose M.; Blanco-Brieva, Gema; Fierro, Jose L. G.
  • Angewandte Chemie International Edition, Vol. 45, Issue 42
  • DOI: 10.1002/anie.200503779

Direct synthesis of hydrogen peroxide from hydrogen and oxygen: An overview of recent developments in the process
journal, November 2008


Advances in the direct synthesis of hydrogen peroxide from hydrogen and oxygen
journal, June 2015


Trends in Selective Hydrogen Peroxide Production on Transition Metal Surfaces from First Principles
journal, November 2012

  • Rankin, Rees B.; Greeley, Jeffrey
  • ACS Catalysis, Vol. 2, Issue 12
  • DOI: 10.1021/cs3003337

Direct synthesis of hydrogen peroxide from H2 and O2 using TiO2-supported Au–Pd catalysts
journal, November 2005


Palladium-tin catalysts for the direct synthesis of H2O2 with high selectivity
journal, February 2016


Switching Off Hydrogen Peroxide Hydrogenation in the Direct Synthesis Process
journal, February 2009


Enabling direct H2O2 production through rational electrocatalyst design
journal, November 2013

  • Siahrostami, Samira; Verdaguer-Casadevall, Arnau; Karamad, Mohammadreza
  • Nature Materials, Vol. 12, Issue 12
  • DOI: 10.1038/nmat3795

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
  • DOI: 10.1021/nl500037x

Mesoporous Nitrogen-Doped Carbon for the Electrocatalytic Synthesis of Hydrogen Peroxide
journal, February 2012

  • Fellinger, Tim-Patrick; Hasché, Frédéric; Strasser, Peter
  • Journal of the American Chemical Society, Vol. 134, Issue 9
  • DOI: 10.1021/ja300038p

Hydrogen Peroxide Synthesis via Enhanced Two-Electron Oxygen Reduction Pathway on Carbon-Coated Pt Surface
journal, December 2014

  • Choi, Chang Hyuck; Kwon, Han Chang; Yook, Sunwoo
  • The Journal of Physical Chemistry C, Vol. 118, Issue 51
  • DOI: 10.1021/jp5113894

Highly Selective Two-Electron Oxygen Reduction Catalyzed by Mesoporous Nitrogen-Doped Carbon
journal, September 2014

  • Park, Jisung; Nabae, Yuta; Hayakawa, Teruaki
  • ACS Catalysis, Vol. 4, Issue 10
  • DOI: 10.1021/cs5008206

Tuning selectivity of electrochemical reactions by atomically dispersed platinum catalyst
journal, March 2016

  • Choi, Chang Hyuck; Kim, Minho; Kwon, Han Chang
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms10922

Tandem cathode for proton exchange membrane fuel cells
journal, January 2013

  • Siahrostami, Samira; Björketun, Mårten E.; Strasser, Peter
  • Physical Chemistry Chemical Physics, Vol. 15, Issue 23
  • DOI: 10.1039/c3cp51479j

Low overpotential water oxidation to hydrogen peroxide on a MnOx catalyst
journal, January 2012

  • Izgorodin, Alex; Izgorodina, Ekaterina; MacFarlane, Douglas R.
  • Energy & Environmental Science, Vol. 5, Issue 11
  • DOI: 10.1039/c2ee21832a

Ion effects in water oxidation to hydrogen peroxide
journal, January 2014

  • McDonnell-Worth, Ciaran; MacFarlane, Douglas. R.
  • RSC Advances, Vol. 4, Issue 58
  • DOI: 10.1039/C4RA05296J

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
  • DOI: 10.1021/acs.jpclett.5b02178

Photocatalytic reactivity for O2− and OH radical formation in anatase and rutile TiO2 suspension as the effect of H2O2 addition
journal, May 2007


Effect of copper ions on the formation of hydrogen peroxide from photocatalytic titanium dioxide particles
journal, October 2003


Quantitative Detection of OH Radicals for Investigating the Reaction Mechanism of Various Visible-Light TiO 2 Photocatalysts in Aqueous Suspension
journal, January 2013

  • Zhang, Jie; Nosaka, Yoshio
  • The Journal of Physical Chemistry C, Vol. 117, Issue 3
  • DOI: 10.1021/jp3105166

Sunscreens as a Source of Hydrogen Peroxide Production in Coastal Waters
journal, August 2014

  • Sánchez-Quiles, David; Tovar-Sánchez, Antonio
  • Environmental Science & Technology, Vol. 48, Issue 16
  • DOI: 10.1021/es5020696

New Insights Into BiVO 4 Properties as Visible Light Photocatalyst
journal, June 2015

  • Saison, Tamar; Chemin, Nicolas; Chanéac, Corinne
  • The Journal of Physical Chemistry C, Vol. 119, Issue 23
  • DOI: 10.1021/acs.jpcc.5b01468

Combined Charge Carrier Transport and Photoelectrochemical Characterization of BiVO 4 Single Crystals: Intrinsic Behavior of a Complex Metal Oxide
journal, July 2013

  • Rettie, Alexander J. E.; Lee, Heung Chan; Marshall, Luke G.
  • Journal of the American Chemical Society, Vol. 135, Issue 30
  • DOI: 10.1021/ja405550k

Enhanced photocatalytic activity of BiVO4 by co-grafting of metal ions and combining with CuBi2O4
journal, June 2013


Electrochemical waste water treatment using high overvoltage anodes Part II: Anode performance and applications
journal, February 1991

  • Stucki, S.; K�tz, R.; Carcer, B.
  • Journal of Applied Electrochemistry, Vol. 21, Issue 2
  • DOI: 10.1007/BF01464288

Electrochemistry and environment: The role of electrocatalysis*1
journal, October 1995


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
  • DOI: 10.1021/jp047349j

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
  • DOI: 10.1002/cctc.201000397

Theoretical evaluation of the surface electrochemistry of perovskites with promising photon absorption properties for solar water splitting
journal, January 2015

  • Montoya, Joseph H.; Garcia-Mota, Monica; Nørskov, Jens K.
  • Physical Chemistry Chemical Physics, Vol. 17, Issue 4
  • DOI: 10.1039/C4CP05259E

A Computational Study of the Hydration of the OH Radical
journal, October 2002

  • Hamad, S.; Lago, S.; Mejías, J. A.
  • The Journal of Physical Chemistry A, Vol. 106, Issue 39
  • DOI: 10.1021/jp013531y

Molecular dynamics study of the hydration of the hydroxyl radical at body temperature
journal, January 2011

  • Pabis, Anna; Szala-Bilnik, Joanna; Swiatla-Wojcik, Dorota
  • Physical Chemistry Chemical Physics, Vol. 13, Issue 20
  • DOI: 10.1039/c0cp02735a

The hydration of the OH radical: Microsolvation modeling and statistical mechanics simulation
journal, October 2003

  • Cabral do Couto, P.; Guedes, R. C.; Costa Cabral, B. J.
  • The Journal of Chemical Physics, Vol. 119, Issue 14
  • DOI: 10.1063/1.1605939

Electrolysis of water on oxide surfaces
journal, September 2007


Universality in Oxygen Reduction Electrocatalysis on Metal Surfaces
journal, July 2012

  • Viswanathan, Venkatasubramanian; Hansen, Heine Anton; Rossmeisl, Jan
  • ACS Catalysis, Vol. 2, Issue 8
  • DOI: 10.1021/cs300227s

Photocatalysts with internal electric fields
journal, January 2014

  • Li, Li; Salvador, Paul A.; Rohrer, Gregory S.
  • Nanoscale, Vol. 6, Issue 1
  • DOI: 10.1039/C3NR03998F

Synthesis and Activities of Rutile IrO 2 and RuO 2 Nanoparticles for Oxygen Evolution in Acid and Alkaline Solutions
journal, January 2012

  • Lee, Youngmin; Suntivich, Jin; May, Kevin J.
  • The Journal of Physical Chemistry Letters, Vol. 3, Issue 3
  • DOI: 10.1021/jz2016507

Oxygen evolution reaction on IrO2-based DSA® type electrodes: kinetics analysis of Tafel lines and EIS
journal, July 2004


Nanosized IrO2 electrocatalysts for oxygen evolution reaction in an SPE electrolyzer
journal, April 2010


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
  • DOI: 10.1021/jp511426q

Oxidation energies of transition metal oxides within the GGA + U framework
journal, May 2006


Works referencing / citing this record:

Quantification of the Charge Consuming Phenomena under High‐Voltage Hold of Carbon/Carbon Supercapacitors by Coupling Operando and Post‐Mortem Analyses
journal, October 2019

  • Przygocki, Patryk; Ratajczak, Paula; Béguin, François
  • Angewandte Chemie, Vol. 131, Issue 50
  • DOI: 10.1002/ange.201907914

Solar‐Driven Production of Hydrogen Peroxide from Water and Dioxygen
journal, February 2018

  • Fukuzumi, Shunichi; Lee, Yong‐Min; Nam, Wonwoo
  • Chemistry – A European Journal, Vol. 24, Issue 20
  • DOI: 10.1002/chem.201704512

The roles of oxygen vacancies, electrolyte composition, lattice structure, and doping density on the electrochemical reactivity of Magnéli phase TiO 2 anodes
journal, January 2018

  • Jing, Yin; Almassi, Soroush; Mehraeen, Shafigh
  • Journal of Materials Chemistry A, Vol. 6, Issue 46
  • DOI: 10.1039/c8ta03719a

Highly durable photoelectrochemical H 2 O 2 production via dual photoanode and cathode processes under solar simulating and external bias-free conditions
journal, January 2020

  • Jeon, Tae Hwa; Kim, Hyejin; Kim, Hyoung-il
  • Energy & Environmental Science, Vol. 13, Issue 6
  • DOI: 10.1039/c9ee03154e

Light-Driven BiVO 4 -C Fuel Cell with Simultaneous Production of H 2 O 2
journal, June 2018

  • Shi, Xinjian; Zhang, Yirui; Siahrostami, Samira
  • Advanced Energy Materials, Vol. 8, Issue 23
  • DOI: 10.1002/aenm.201801158

Quantifying robustness of DFT predicted pathways and activity determining elementary steps for electrochemical reactions
journal, January 2019

  • Krishnamurthy, Dilip; Sumaria, Vaidish; Viswanathan, Venkatasubramanian
  • The Journal of Chemical Physics, Vol. 150, Issue 4
  • DOI: 10.1063/1.5056167

Electrochemical Carbon Dioxide Splitting
journal, February 2019


Photocatalytic 4-nitrophenol degradation and oxygen evolution reaction in CuO/g-C 3 N 4 composites prepared by deep eutectic solvent-assisted chlorine doping
journal, January 2019

  • Verma, Atul; Jaihindh, Dhayanantha Prabu; Fu, Yen-Pei
  • Dalton Transactions, Vol. 48, Issue 24
  • DOI: 10.1039/c9dt01046g

Selective Electrochemical H 2 O 2 Production through Two-Electron Oxygen Electrochemistry
journal, September 2018

  • Jiang, Yuanyuan; Ni, Pengjuan; Chen, Chuanxia
  • Advanced Energy Materials, Vol. 8, Issue 31
  • DOI: 10.1002/aenm.201801909

A highly efficient photoelectrochemical H 2 O 2 production reaction with Co 3 O 4 as a co-catalyst
journal, January 2018

  • Zhang, Jijie; Chang, Xiaoxia; Luo, Zhibin
  • Chemical Communications, Vol. 54, Issue 51
  • DOI: 10.1039/c8cc03303j

Quantification of the Charge Consuming Phenomena under High‐Voltage Hold of Carbon/Carbon Supercapacitors by Coupling Operando and Post‐Mortem Analyses
journal, December 2019

  • Przygocki, Patryk; Ratajczak, Paula; Béguin, François
  • Angewandte Chemie International Edition, Vol. 58, Issue 50
  • DOI: 10.1002/anie.201907914

Electrochemical synthesis of hydrogen peroxide from water and oxygen
journal, June 2019

  • Perry, Samuel C.; Pangotra, Dhananjai; Vieira, Luciana
  • Nature Reviews Chemistry, Vol. 3, Issue 7
  • DOI: 10.1038/s41570-019-0110-6

Understanding activity trends in electrochemical water oxidation to form hydrogen peroxide
journal, September 2017


Harvesting multiple electron–hole pairs generated through plasmonic excitation of Au nanoparticles
journal, May 2018


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
  • DOI: 10.1039/c9ta12468c

Understanding activity trends in electrochemical water oxidation to form hydrogen peroxide
text, January 2017