skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Engineering Active Fe Sites on Nickel–Iron Layered Double Hydroxide through Component Segregation for Oxygen Evolution Reaction

Abstract

Nickel-iron layered double hydroxide (NiFe LDH) is a promising oxygen evolution reaction (OER) electrocatalyst under alkaline conditions. Much research has been performed to understand the structure-activity relationship of NiFe LDH under OER conditions. However, the specific role of the Fe species remains unclear and under debate. Herein, based on DFT calculations, it was discovered that the edge Fe sites show higher activity towards OER than either the edge Ni sites or lattice sites. Therefore, a facile acid-etching method was proposed to controllably induce the formation of edge Fe sites in NiFe LDH, and the obtained sample exhibited higher OER activity. X-ray absorption near edge structure and extended X-ray absorption fine structure analyses further revealed that the interaction of the edge Fe species with Ni is believed to contribute to the enhancement of the OER performance. This work provides a new understanding of the structure-activity relationship in NiFe LDH and offers a facile method for the design of efficient electrocatalysts in an alkaline environment.

Authors:
 [1];  [1];  [2];  [1];  [1];  [3];  [4];  [2];  [5]; ORCiD logo [2]
  1. Chinese Academy of Sciences (CAS), Shanghai (China). Shanghai Inst. of Ceramics, State Key Lab. of High Perf. Ceramics and Superfine Microstructure, and Center of Materials Science and Optoelectronics Engineering
  2. Chinese Academy of Sciences (CAS), Shanghai (China). Shanghai Inst. of Ceramics, State Key Lab. of High Perf. Ceramics and Superfine Microstructure
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  5. Univ. of Queensland, Brisbane, QLD (Australia). Nanomaterials Centre, School of Chemical Engineering and Australian Inst. for Bioengineering and Nanotechnology
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Natural Science Foundation of China (NNSFC); USDOE Office of Science (SC)
OSTI Identifier:
1632119
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ChemSusChem
Additional Journal Information:
Journal Volume: 13; Journal Issue: 4; Journal ID: ISSN 1864-5631
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; electrocatalysis; layered double hydroxide; nanosheet; oxygen evolution reaction; water splitting

Citation Formats

Peng, Chunlei, Ran, Nian, Wan, Gang, Zhao, Wanpeng, Kuang, Zhaoyu, Lu, Zheng, Sun, Chengjun, Liu, Jianjun, Wang, Lianzhou, and Chen, Hangrong. Engineering Active Fe Sites on Nickel–Iron Layered Double Hydroxide through Component Segregation for Oxygen Evolution Reaction. United States: N. p., 2020. Web. https://doi.org/10.1002/cssc.201902841.
Peng, Chunlei, Ran, Nian, Wan, Gang, Zhao, Wanpeng, Kuang, Zhaoyu, Lu, Zheng, Sun, Chengjun, Liu, Jianjun, Wang, Lianzhou, & Chen, Hangrong. Engineering Active Fe Sites on Nickel–Iron Layered Double Hydroxide through Component Segregation for Oxygen Evolution Reaction. United States. https://doi.org/10.1002/cssc.201902841
Peng, Chunlei, Ran, Nian, Wan, Gang, Zhao, Wanpeng, Kuang, Zhaoyu, Lu, Zheng, Sun, Chengjun, Liu, Jianjun, Wang, Lianzhou, and Chen, Hangrong. Tue . "Engineering Active Fe Sites on Nickel–Iron Layered Double Hydroxide through Component Segregation for Oxygen Evolution Reaction". United States. https://doi.org/10.1002/cssc.201902841. https://www.osti.gov/servlets/purl/1632119.
@article{osti_1632119,
title = {Engineering Active Fe Sites on Nickel–Iron Layered Double Hydroxide through Component Segregation for Oxygen Evolution Reaction},
author = {Peng, Chunlei and Ran, Nian and Wan, Gang and Zhao, Wanpeng and Kuang, Zhaoyu and Lu, Zheng and Sun, Chengjun and Liu, Jianjun and Wang, Lianzhou and Chen, Hangrong},
abstractNote = {Nickel-iron layered double hydroxide (NiFe LDH) is a promising oxygen evolution reaction (OER) electrocatalyst under alkaline conditions. Much research has been performed to understand the structure-activity relationship of NiFe LDH under OER conditions. However, the specific role of the Fe species remains unclear and under debate. Herein, based on DFT calculations, it was discovered that the edge Fe sites show higher activity towards OER than either the edge Ni sites or lattice sites. Therefore, a facile acid-etching method was proposed to controllably induce the formation of edge Fe sites in NiFe LDH, and the obtained sample exhibited higher OER activity. X-ray absorption near edge structure and extended X-ray absorption fine structure analyses further revealed that the interaction of the edge Fe species with Ni is believed to contribute to the enhancement of the OER performance. This work provides a new understanding of the structure-activity relationship in NiFe LDH and offers a facile method for the design of efficient electrocatalysts in an alkaline environment.},
doi = {10.1002/cssc.201902841},
journal = {ChemSusChem},
number = 4,
volume = 13,
place = {United States},
year = {2020},
month = {1}
}

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

Citation Metrics:
Cited by: 3 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Operando Analysis of NiFe and Fe Oxyhydroxide Electrocatalysts for Water Oxidation: Detection of Fe 4+ by Mössbauer Spectroscopy
journal, November 2015

  • Chen, Jamie Y. C.; Dang, Lianna; Liang, Hanfeng
  • Journal of the American Chemical Society, Vol. 137, Issue 48
  • DOI: 10.1021/jacs.5b10699

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Fluoridated Iron–Nickel Layered Double Hydroxide for Enhanced Performance in the Oxygen Evolution Reaction
journal, July 2019


An investigation of phase transitions in rust layers using raman spectroscopy
journal, January 1989


Introducing Fe 2+ into Nickel-Iron Layered Double Hydroxide: Local Structure Modulated Water Oxidation Activity
journal, June 2018


Projector augmented-wave method
journal, December 1994


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

Abundance and distribution of palladium, platinum, iridium and gold in some oxide minerals
journal, February 1984


Hydrogen and fuel cells: Towards a sustainable energy future
journal, December 2008


Effects of Fe Electrolyte Impurities on Ni(OH) 2 /NiOOH Structure and Oxygen Evolution Activity
journal, March 2015

  • Klaus, Shannon; Cai, Yun; Louie, Mary W.
  • The Journal of Physical Chemistry C, Vol. 119, Issue 13
  • DOI: 10.1021/acs.jpcc.5b00105

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
  • DOI: 10.1021/ja405351s

Oxygen reduction and evolution at single-metal active sites: Comparison between functionalized graphitic materials and protoporphyrins
journal, January 2013


Introducing Fe 2+ into Nickel-Iron Layered Double Hydroxide: Local Structure Modulated Water Oxidation Activity
journal, June 2018

  • Cai, Zhao; Zhou, Daojin; Wang, Maoyu
  • Angewandte Chemie International Edition, Vol. 57, Issue 30
  • DOI: 10.1002/anie.201804881

Hexagonal nanosheets from the exfoliation of Ni2+-Fe3+ LDHs: a route towards layered multifunctional materials
journal, January 2010

  • Abellán, Gonzalo; Coronado, Eugenio; Martí-Gastaldo, Carlos
  • Journal of Materials Chemistry, Vol. 20, Issue 35
  • DOI: 10.1039/c0jm01447h

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


An ethylene glycol intercalated monometallic layered double hydroxide based on iron as an efficient bifunctional catalyst
journal, January 2016

  • Nagarajan, Rajamani; Gupta, Pankaj; Singh, Poonam
  • Dalton Transactions, Vol. 45, Issue 43
  • DOI: 10.1039/C6DT03129C

NiFe Hydroxide Lattice Tensile Strain: Enhancement of Adsorption of Oxygenated Intermediates for Efficient Water Oxidation Catalysis
journal, December 2018


Synergy between Fe and Ni in the optimal performance of (Ni,Fe)OOH catalysts for the oxygen evolution reaction
journal, May 2018

  • Xiao, Hai; Shin, Hyeyoung; Goddard, William A.
  • Proceedings of the National Academy of Sciences, Vol. 115, Issue 23
  • DOI: 10.1073/pnas.1722034115

The Catalysis of the Oxygen Evolution Reaction by Iron Impurities in Thin Film Nickel Oxide Electrodes
journal, January 1987

  • Corrigan, Dennis A.
  • Journal of The Electrochemical Society, Vol. 134, Issue 2
  • DOI: 10.1149/1.2100463

Trapping an Iron(VI) Water-Splitting Intermediate in Nonaqueous Media
journal, April 2018


NiFe-Based (Oxy)hydroxide Catalysts for Oxygen Evolution Reaction in Non-Acidic Electrolytes
journal, July 2016


Catalytic applications of layered double hydroxides: recent advances and perspectives
journal, January 2014

  • Fan, Guoli; Li, Feng; Evans, David G.
  • Chem. Soc. Rev., Vol. 43, Issue 20
  • DOI: 10.1039/C4CS00160E

An Advanced Ni–Fe Layered Double Hydroxide Electrocatalyst for Water Oxidation
journal, May 2013

  • Gong, Ming; Li, Yanguang; Wang, Hailiang
  • Journal of the American Chemical Society, Vol. 135, Issue 23
  • DOI: 10.1021/ja4027715

Oxygen Evolution Reaction Dynamics, Faradaic Charge Efficiency, and the Active Metal Redox States of Ni–Fe Oxide Water Splitting Electrocatalysts
journal, April 2016

  • Görlin, Mikaela; Chernev, Petko; Ferreira de Araújo, Jorge
  • Journal of the American Chemical Society, Vol. 138, Issue 17
  • DOI: 10.1021/jacs.6b00332

Single-Atom Au/NiFe Layered Double Hydroxide Electrocatalyst: Probing the Origin of Activity for Oxygen Evolution Reaction
journal, February 2018

  • Zhang, Jingfang; Liu, Jieyu; Xi, Lifei
  • Journal of the American Chemical Society, Vol. 140, Issue 11
  • DOI: 10.1021/jacs.8b00752

Identification of Highly Active Fe Sites in (Ni,Fe)OOH for Electrocatalytic Water Splitting
journal, January 2015

  • Friebel, Daniel; Louie, Mary W.; Bajdich, Michal
  • Journal of the American Chemical Society, Vol. 137, Issue 3
  • DOI: 10.1021/ja511559d

High-Performance Pyrochlore-Type Yttrium Ruthenate Electrocatalyst for Oxygen Evolution Reaction in Acidic Media
journal, August 2017

  • Kim, Jaemin; Shih, Pei-Chieh; Tsao, Kai-Chieh
  • Journal of the American Chemical Society, Vol. 139, Issue 34
  • DOI: 10.1021/jacs.7b06808

Reactive Fe-Sites in Ni/Fe (Oxy)hydroxide Are Responsible for Exceptional Oxygen Electrocatalysis Activity
journal, August 2017

  • Stevens, Michaela Burke; Trang, Christina D. M.; Enman, Lisa J.
  • Journal of the American Chemical Society, Vol. 139, Issue 33
  • DOI: 10.1021/jacs.7b07117

Semiempirical GGA-type density functional constructed with a long-range dispersion correction
journal, January 2006

  • Grimme, Stefan
  • Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799
  • DOI: 10.1002/jcc.20495

Nickel–Iron Oxyhydroxide Oxygen-Evolution Electrocatalysts: The Role of Intentional and Incidental Iron Incorporation
journal, April 2014

  • Trotochaud, Lena; Young, Samantha L.; Ranney, James K.
  • Journal of the American Chemical Society, Vol. 136, Issue 18
  • DOI: 10.1021/ja502379c

Atomically dispersed nickel–nitrogen–sulfur species anchored on porous carbon nanosheets for efficient water oxidation
journal, March 2019


NiFe Hydroxide Lattice Tensile Strain: Enhancement of Adsorption of Oxygenated Intermediates for Efficient Water Oxidation Catalysis
journal, December 2018

  • Zhou, Daojin; Wang, Shiyuan; Jia, Yin
  • Angewandte Chemie International Edition, Vol. 58, Issue 3
  • DOI: 10.1002/anie.201809689

Breaking Long-Range Order in Iridium Oxide by Alkali Ion for Efficient Water Oxidation
journal, January 2019

  • Gao, Jiajian; Xu, Cong-Qiao; Hung, Sung-Fu
  • Journal of the American Chemical Society, Vol. 141, Issue 7
  • DOI: 10.1021/jacs.8b11456

Hierarchical Hollow Nanoprisms Based on Ultrathin Ni-Fe Layered Double Hydroxide Nanosheets with Enhanced Electrocatalytic Activity towards Oxygen Evolution
journal, December 2017

  • Yu, Le; Yang, Jing Fan; Guan, Bu Yuan
  • Angewandte Chemie International Edition, Vol. 57, Issue 1
  • DOI: 10.1002/anie.201710877

Influence of iron doping on tetravalent nickel content in catalytic oxygen evolving films
journal, January 2017

  • Li, Nancy; Bediako, D. Kwabena; Hadt, Ryan G.
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 7
  • DOI: 10.1073/pnas.1620787114

Three-dimensional NiFe layered double hydroxide film for high-efficiency oxygen evolution reaction
journal, January 2014

  • Lu, Zhiyi; Xu, Wenwen; Zhu, Wei
  • Chem. Commun., Vol. 50, Issue 49
  • DOI: 10.1039/C4CC01625D

FeN 4 Sites Embedded into Carbon Nanofiber Integrated with Electrochemically Exfoliated Graphene for Oxygen Evolution in Acidic Medium
journal, August 2018

  • Lei, Chaojun; Chen, Hengquan; Cao, Junhui
  • Advanced Energy Materials, Vol. 8, Issue 26
  • DOI: 10.1002/aenm.201801912

A universal principle for a rational design of single-atom electrocatalysts
journal, April 2018