Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Dynamic stability of active sites in hydr(oxy)oxides for the oxygen evolution reaction

Journal Article · · Nature Energy
The poor activity and stability of electrode materials for the oxygen evolution reaction are the main bottlenecks in the water-splitting reaction for H2 production. In this work, by studying the activity–stability trends for the oxygen evolution reaction on conductive M1OxHy, Fe–M1OxHy and Fe–M1M2OxHy hydr(oxy)oxide clusters (M1 = Ni, Co, Fe; M2 = Mn, Co, Cu), we show that balancing the rates of Fe dissolution and redeposition over a MOxHy host establishes dynamically stable Fe active sites. Together with tuning the Fe content of the electrolyte, the strong interaction of Fe with the MOxHy host is the key to controlling the average number of Fe active sites present at the solid/liquid interface. We suggest that the Fe–M adsorption energy can therefore serve as a reaction descriptor that unifies oxygen evolution reaction catalysis on 3d transition-metal hydr(oxy)oxides in alkaline media. Thus, the introduction of dynamically stable active sites extends the design rules for creating active and stable interfaces.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS) and Center for Nanoscale Materials (CNM)
Sponsoring Organization:
Japan Society for the Promotion of Science (JSPS); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1632277
Journal Information:
Nature Energy, Journal Name: Nature Energy Journal Issue: 3 Vol. 5; ISSN 2058-7546
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (67)

NiFe-Based (Oxy)hydroxide Catalysts for Oxygen Evolution Reaction in Non-Acidic Electrolytes journal July 2016
Recent Progress on Multimetal Oxide Catalysts for the Oxygen Evolution Reaction journal January 2018
Using Surface Segregation To Design Stable Ru-Ir Oxides for the Oxygen Evolution Reaction in Acidic Environments journal October 2014
Chemical Recognition of Active Oxygen Species on the Surface of Oxygen Evolution Reaction Electrocatalysts journal June 2017
Enhancement of Oxygen Evolution Activity of Nickel Oxyhydroxide by Electrolyte Alkali Cations journal July 2019
Using Surface Segregation To Design Stable Ru-Ir Oxides for the Oxygen Evolution Reaction in Acidic Environments journal October 2014
Chemical Recognition of Active Oxygen Species on the Surface of Oxygen Evolution Reaction Electrocatalysts journal June 2017
Enhancement of Oxygen Evolution Activity of Nickel Oxyhydroxide by Electrolyte Alkali Cations journal July 2019
Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces journal March 2011
Benchmarking the Stability of Oxygen Evolution Reaction Catalysts: The Importance of Monitoring Mass Losses journal October 2014
Semiempirical GGA-type density functional constructed with a long-range dispersion correction journal January 2006
Improved grid-based algorithm for Bader charge allocation journal January 2007
Osmium nanoislands spontaneously deposited on a Pt(111) electrode: an XPS, STM and GIF-XAS study journal September 2003
Electrolysis of water on oxide surfaces journal September 2007
Oxygen Evolution Reaction Electrocatalysis on Transition Metal Oxides and (Oxy)hydroxides: Activity Trends and Design Principles journal October 2015
Fe (Oxy)hydroxide Oxygen Evolution Reaction Electrocatalysis: Intrinsic Activity and the Roles of Electrical Conductivity, Substrate, and Dissolution journal November 2015
Revised Oxygen Evolution Reaction Activity Trends for First-Row Transition-Metal (Oxy)hydroxides in Alkaline Media journal August 2015
Guidelines for the Rational Design of Ni-Based Double Hydroxide Electrocatalysts for the Oxygen Evolution Reaction journal August 2015
Relationships between Atomic Level Surface Structure and Stability/Activity of Platinum Surface Atoms in Aqueous Environments journal March 2016
Oxygen Evolution Reaction—The Enigma in Water Electrolysis journal September 2018
An Unconventional Iron Nickel Catalyst for the Oxygen Evolution Reaction journal February 2019
Benchmarking Heterogeneous Electrocatalysts for the Oxygen Evolution Reaction journal October 2013
A Functionally Stable Manganese Oxide Oxygen Evolution Catalyst in Acid journal April 2014
Nickel–Iron Oxyhydroxide Oxygen-Evolution Electrocatalysts: The Role of Intentional and Incidental Iron Incorporation journal April 2014
Identification of Highly Active Fe Sites in (Ni,Fe)OOH for Electrocatalytic Water Splitting journal January 2015
A Self-Healing Oxygen-Evolving Catalyst journal March 2009
Operando Analysis of NiFe and Fe Oxyhydroxide Electrocatalysts for Water Oxidation: Detection of Fe 4+ by Mössbauer Spectroscopy journal November 2015
Oxygen Evolution Reaction Dynamics, Faradaic Charge Efficiency, and the Active Metal Redox States of Ni–Fe Oxide Water Splitting Electrocatalysts journal April 2016
Reactive Fe-Sites in Ni/Fe (Oxy)hydroxide Are Responsible for Exceptional Oxygen Electrocatalysis Activity journal August 2017
Origin of Anomalous Activities for Electrocatalysts in Alkaline Electrolytes journal October 2012
Activity Descriptors for CO 2 Electroreduction to Methane on Transition-Metal Catalysts journal January 2012
Activity–Stability Trends for the Oxygen Evolution Reaction on Monometallic Oxides in Acidic Environments journal July 2014
Time-resolved observations of water oxidation intermediates on a cobalt oxide nanoparticle catalyst journal February 2014
Activating lattice oxygen redox reactions in metal oxides to catalyse oxygen evolution journal January 2017
The role of non-covalent interactions in electrocatalytic fuel-cell reactions on platinum journal August 2009
Water electrolysis on La1−xSrxCoO3−δ perovskite electrocatalysts journal March 2016
Functional links between stability and reactivity of strontium ruthenate single crystals during oxygen evolution journal June 2014
Stabilization of ultrathin (hydroxy)oxide films on transition metal substrates for electrochemical energy conversion journal May 2017
Trends in activity for the water electrolyser reactions on 3d M(Ni,Co,Fe,Mn) hydr(oxy)oxide catalysts journal May 2012
Energy and fuels from electrochemical interfaces journal December 2016
Dynamic surface self-reconstruction is the key of highly active perovskite nano-electrocatalysts for water splitting journal July 2017
Balancing activity, stability and conductivity of nanoporous core-shell iridium/iridium oxide oxygen evolution catalysts journal November 2017
Voltage- and time-dependent valence state transition in cobalt oxide catalysts during the oxygen evolution reaction journal April 2020
Chemical and structural origin of lattice oxygen oxidation in Co–Zn oxyhydroxide oxygen evolution electrocatalysts journal March 2019
Key role of chemistry versus bias in electrocatalytic oxygen evolution journal November 2020
The stability number as a metric for electrocatalyst stability benchmarking journal June 2018
Impact of nanoparticle size and lattice oxygen on water oxidation on NiFeOxHy journal November 2018
Thermodynamic explanation of the universal correlation between oxygen evolution activity and corrosion of oxide catalysts journal July 2015
Reaction chemistry in rechargeable Li–O 2 batteries journal January 2017
Parameter-free calculations of X-ray spectra with FEFF9 journal January 2010
Implicit solvation model for density-functional study of nanocrystal surfaces and reaction pathways journal February 2014
Implicit self-consistent electrolyte model in plane-wave density-functional theory journal December 2019
Influence of iron doping on tetravalent nickel content in catalytic oxygen evolving films journal January 2017
Characterization of NiFe oxyhydroxide electrocatalysts by integrated electronic structure calculations and spectroelectrochemistry journal March 2017
Synergy between Fe and Ni in the optimal performance of (Ni,Fe)OOH catalysts for the oxygen evolution reaction journal May 2018
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study journal January 1998
Generalized Gradient Approximation Made Simple journal October 1996
In situ formation of molecular Ni-Fe active sites on heteroatom-doped graphene as a heterogeneous electrocatalyst toward oxygen evolution journal March 2018
Enhancing Hydrogen Evolution Activity in Water Splitting by Tailoring Li+-Ni(OH)2-Pt Interfaces journal December 2011
A Perovskite Oxide Optimized for Oxygen Evolution Catalysis from Molecular Orbital Principles journal October 2011
A Reversible and Higher-Rate Li-O2 Battery journal July 2012
Combining theory and experiment in electrocatalysis: Insights into materials design journal January 2017
Homogeneously dispersed multimetal oxygen-evolving catalysts journal March 2016
A highly active and stable IrO x /SrIrO 3 catalyst for the oxygen evolution reaction journal September 2016
The Catalysis of the Oxygen Evolution Reaction by Iron Impurities in Thin Film Nickel Oxide Electrodes journal January 1987
Thermodynamic explanation of the universal correlation between oxygen evolution activity and corrosion of oxide catalysts text January 2015

Similar Records

Dynamically Stable Active Sites from Surface Evolution of Perovskite Materials during the Oxygen Evolution Reaction
Journal Article · Mon Jan 04 19:00:00 EST 2021 · Journal of the American Chemical Society · OSTI ID:1774576

Trends in activity for the water electrolyzer reactions on 3d-M(Ni,Co,Fe,Mn)-hydr(oxy)oxide catalysts.
Journal Article · Sat Dec 31 23:00:00 EST 2011 · Nature Materials · OSTI ID:1050179

Operando X‐Ray Absorption Spectroscopy Shows Iron Oxidation Is Concurrent with Oxygen Evolution in Cobalt–Iron (Oxy)hydroxide Electrocatalysts
Journal Article · Mon Sep 03 20:00:00 EDT 2018 · Angewandte Chemie · OSTI ID:1468491