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Introducing Fe2+ into Nickel-Iron Layered Double Hydroxide: Local Structure Modulated Water Oxidation Activity

Journal Article · · Angewandte Chemie (International Edition)
 [1];  [2];  [3];  [4];  [5];  [5];  [2];  [2];  [2];  [1];  [6];  [2];  [4];  [7];  [3];  [5];  [2]
  1. Beijing Univ. of Chemical Technology, Beijing (China); Yale Univ., New Haven, CT (United States)
  2. Beijing Univ. of Chemical Technology, Beijing (China)
  3. Oregon State Univ., Corvallis, OR (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States)
  5. Yale Univ., New Haven, CT (United States)
  6. Stanford Univ., Stanford, CA (United States)
  7. Univ. of Oxford, Oxford (United Kingdom)
Exploring materials with regulated local structures and understanding how the atomic motifs govern the reactivity and durability of catalysts are a critical challenge for designing advanced catalysts. Here we report the tuning of the local atomic structure of nickel–iron layered double hydroxides (NiFe–LDHs) by partially substituting Ni2+ with Fe2+ to introduce Fe–O–Fe moieties. These Fe2+–containing NiFe–LDHs exhibit enhanced oxygen evolution reaction (OER) activity with an ultralow overpotential of 195 mV at the current density of 10 mA/cm2, which is among the best OER catalytic performance reported to date. In–situ X–ray absorption, Raman, and electrochemical analysis jointly reveal that the Fe–O–Fe motifs could stabilize high–valent metal sites at low overpotentials, thereby enhancing the OER activity. Lastly, these results reveal the importance of tuning the local atomic structure for designing high efficiency electrocatalysts.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Grant/Contract Number:
SC0012704
OSTI ID:
1454823
Alternate ID(s):
OSTI ID: 1457470
OSTI ID: 1470489
Report Number(s):
BNL--205757-2018-JAAM
Journal Information:
Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 30 Vol. 57; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

References (34)

Hierarchical NiMn Layered Double Hydroxide/Carbon Nanotubes Architecture with Superb Energy Density for Flexible Supercapacitors journal January 2014
Spatially Confined Hybridization of Nanometer-Sized NiFe Hydroxides into Nitrogen-Doped Graphene Frameworks Leading to Superior Oxygen Evolution Reactivity journal June 2015
NiFe-Based (Oxy)hydroxide Catalysts for Oxygen Evolution Reaction in Non-Acidic Electrolytes journal July 2016
Single-Crystalline Ultrathin Co 3 O 4 Nanosheets with Massive Vacancy Defects for Enhanced Electrocatalysis journal September 2017
Hierarchical Hollow Nanoprisms Based on Ultrathin Ni-Fe Layered Double Hydroxide Nanosheets with Enhanced Electrocatalytic Activity towards Oxygen Evolution journal December 2017
Hierarchical Hollow Nanoprisms Based on Ultrathin Ni-Fe Layered Double Hydroxide Nanosheets with Enhanced Electrocatalytic Activity towards Oxygen Evolution journal December 2017
Active Sites in Fe/MFI Catalysts for NOx Reduction and Oscillating N2O Decomposition journal December 2000
X-ray absorption spectroscopy to analyze nuclear geometry and electronic structure of biological metal centers?potential and questions examined with special focus on the tetra-nuclear manganese complex of oxygenic photosynthesis journal July 2003
Redox topotactic reactions in Fe II −  III (oxy)hydroxycarbonate new minerals related to fougèrite in gleysols: “trébeurdenite and mössbauerite” journal January 2012
A mini review of NiFe-based materials as highly active oxygen evolution reaction electrocatalysts journal November 2014
Phosphorus oxoanion-intercalated layered double hydroxides for high-performance oxygen evolution journal February 2017
Analysis of XPS spectra of Fe2+ and Fe3+ ions in oxide materials journal February 2008
Understanding the incorporating effect of Co2+/Co3+ in NiFe-layered double hydroxide for electrocatalytic oxygen evolution reaction journal February 2018
Valence Change Ability and Geometrical Occupation of Substitution Cations Determine the Pseudocapacitance of Spinel Ferrite XFe 2 O 4 (X = Mn, Co, Ni, Fe) journal June 2016
Dual Mechanisms: Hydrogen Transfer during Water Oxidation Catalysis of Pure and Fe-Doped Nickel Oxyhydroxide journal July 2017
Recent Advances in the Synthesis and Application of Layered Double Hydroxide (LDH) Nanosheets journal March 2012
Control of Surface Defects and Agglomeration Mechanism of Layered Double Hydroxide Nanoparticles journal March 2012
Benchmarking Heterogeneous Electrocatalysts for the Oxygen Evolution Reaction journal October 2013
Ultrathin Cobalt–Manganese Layered Double Hydroxide Is an Efficient Oxygen Evolution Catalyst journal November 2014
Identification of Highly Active Fe Sites in (Ni,Fe)OOH for Electrocatalytic Water Splitting journal January 2015
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
Oxidatively Electrodeposited Thin-Film Transition Metal (Oxy)hydroxides as Oxygen Evolution Catalysts journal July 2016
Tracking Catalyst Redox States and Reaction Dynamics in Ni–Fe Oxyhydroxide Oxygen Evolution Reaction Electrocatalysts: The Role of Catalyst Support and Electrolyte pH journal January 2017
Reactive Fe-Sites in Ni/Fe (Oxy)hydroxide Are Responsible for Exceptional Oxygen Electrocatalysis Activity journal August 2017
Single-Atom Au/NiFe Layered Double Hydroxide Electrocatalyst: Probing the Origin of Activity for Oxygen Evolution Reaction journal February 2018
Exfoliation of layered double hydroxides for enhanced oxygen evolution catalysis journal July 2014
Local atomic structure modulations activate metal oxide as electrocatalyst for hydrogen evolution in acidic water journal August 2015
Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction journal January 2018
Catalytic applications of layered double hydroxides: recent advances and perspectives journal January 2014
The secret behind the success of doping nickel oxyhydroxide with iron journal January 2017
O-atom transport catalysis by neutral manganese oxide clusters in the gas phase: Reactions with CO, C 2 H 4 , NO 2 , and O 2 journal August 2013
Mg/Al Ordering in Layered Double Hydroxides Revealed by Multinuclear NMR Spectroscopy journal July 2008
Mechanism of catalytic oxygenation of alkanes by halogenated iron porphyrins journal May 1994

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2D Layered Double Hydroxides for Oxygen Evolution Reaction: From Fundamental Design to Application journal March 2019
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Layered Metal Hydroxides and Their Derivatives: Controllable Synthesis, Chemical Exfoliation, and Electrocatalytic Applications journal November 2019
NiFe Hydroxide Lattice Tensile Strain: Enhancement of Adsorption of Oxygenated Intermediates for Efficient Water Oxidation Catalysis journal December 2018
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Engineering Active Fe Sites on Nickel–Iron Layered Double Hydroxide through Component Segregation for Oxygen Evolution Reaction journal January 2020
Inlaying Ultrathin Bimetallic MOF Nanosheets into 3D Ordered Macroporous Hydroxide for Superior Electrocatalytic Oxygen Evolution journal July 2019
Fe 2+ ‐Doped Layered Double (Ni, Fe) Hydroxides as Efficient Electrocatalysts for Water Splitting and Self‐Powered Electrochemical Systems journal August 2019
Non‐3d Metal Modulation of a 2D Ni–Co Heterostructure Array as Multifunctional Electrocatalyst for Portable Overall Water Splitting journal March 2020
Reducing Oxygen Evolution Reaction Overpotential in Cobalt‐Based Electrocatalysts via Optimizing the “Microparticles‐in‐Spider Web” Electrode Configurations journal January 2020
Co3O4 nanocage derived from metal-organic frameworks: An excellent cathode catalyst for rechargeable Li-O2 battery journal April 2019
Self-magnetic-attracted NixFe(1−x)@NixFe(1−x)O nanoparticles on nickel foam as highly active and stable electrocatalysts towards alkaline oxygen evolution reaction journal January 2020
In Situ X-ray Absorption Spectroscopy Studies of Nanoscale Electrocatalysts journal June 2019
Boosting oxygen evolution of single-atomic ruthenium through electronic coupling with cobalt-iron layered double hydroxides journal April 2019
Structural defects on converted bismuth oxide nanotubes enable highly active electrocatalysis of carbon dioxide reduction journal June 2019
Atomic and electronic modulation of self-supported nickel-vanadium layered double hydroxide to accelerate water splitting kinetics journal August 2019
Aqueous-phase synthesis of layered double hydroxide nanoplates as catalysts for the oxygen evolution reaction journal January 2018
Superaerophilic copper nanowires for efficient and switchable CO 2 electroreduction journal January 2019
Intramolecular electronic coupling in porous iron cobalt (oxy)phosphide nanoboxes enhances the electrocatalytic activity for oxygen evolution journal January 2019
Self-supported Co-doped FeNi carbonate hydroxide nanosheet array as a highly efficient electrocatalyst towards the oxygen evolution reaction in an alkaline solution journal January 2019
In situ growth of layered double hydroxides on boehmite AlOOH for active and stable oxygen evolution in alkaline media journal January 2019
Loading FeOOH on Ni(OH) 2 hollow nanorods to obtain a three-dimensional sandwich catalyst with strong electron interactions for an efficient oxygen evolution reaction journal January 2020
Temperature and doping-tuned coordination environments around electroactive centers in Fe-doped α(β)-Ni(OH) 2 for excellent water splitting journal January 2020
Nanoporous gold supported chromium-doped NiFe oxyhydroxides as high-performance catalysts for the oxygen evolution reaction journal January 2019
Insight into the role of Ni–Fe dual sites in the oxygen evolution reaction based on atomically metal-doped polymeric carbon nitride journal January 2019
Partially delocalized charge in Fe-doped NiCo 2 S 4 nanosheet–mesoporous carbon-composites for high-voltage supercapacitors journal January 2019
Surface evolution and reconstruction of oxygen-abundant FePi/NiFeP synergy in NiFe phosphides for efficient water oxidation journal January 2019
Ultrafast X-ray Absorption Studies of the Structural Dynamics of Molecular and Biological Systems in Solution journal May 2011

Figures / Tables (4)


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