Unraveling Geometrical Site Confinement in Highly Efficient Iron-Doped Electrocatalysts toward Oxygen Evolution Reaction

Sung Fu Hung; Ying Ya Hsu; Chia Jui Chang; Chia Shuo Hsu; Nian Tzu Suen; Ting Shan Chan; Hao Ming Chen

doi:10.1002/aenm.201701686

Unraveling Geometrical Site Confinement in Highly Efficient Iron-Doped Electrocatalysts toward Oxygen Evolution Reaction

Sung Fu Hung, Ying Ya Hsu, Chia Jui Chang, Chia Shuo Hsu, Nian Tzu Suen, Ting Shan Chan, Hao Ming Chen^*

^*Corresponding author for this work

Department of Applied Chemistry

Research output: Contribution to journal › Article › peer-review

157 Scopus citations

Abstract

Introduction of iron in various catalytic systems has served a crucial function to significantly enhance the catalytic activity toward oxygen evolution reaction (OER), but the relationship between material properties and catalysis is still elusive. In this study, by regulating the distinctive geometric sites in spinel, Fe occupies the octahedral sites (Fe³⁺ _(Oh)) and confines Co to the tetrahedral site (Co²⁺ _(Td)), resulting in a strikingly high activity (η_{j = 10 mA cm} ⁻² = 229 mV and η_{j = 100 mA cm} ⁻² = 281 mV). Further enrichment of Fe ions would occupy the tetrahedral sites to decline the amount of Co²⁺ _(Td) and deteriorate the OER activity. It is also found that similar tafel slope and peak frequency in Bode plot of electrochemical impedance spectroscopy indicate that Co²⁺ _(Td) ions are primarily in charge of water oxidation catalytic center. By means of electrochemical techniques and in situ X-ray absorption spectroscopy, it is proposed that Fe³⁺ _(Oh) ions mainly confine cobalt ions to the tetrahedral site to restrain the multipath transfer of cobalt ions during the dynamic structural transformation between spinel and oxyhydroxide, continuously activating the catalytic behavior of Co²⁺ _(Td) ions. This material-related insight provides an indication for the design of highly efficient OER electrocatalysts.

Original language	English
Article number	1701686
Journal	Advanced Energy Materials
Volume	8
Issue number	7
DOIs	https://doi.org/10.1002/aenm.201701686
State	Published - 5 Mar 2018

Keywords

electrocatalysts
highly efficient
iron
oxygen evolution reaction
water splitting

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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title = "Unraveling Geometrical Site Confinement in Highly Efficient Iron-Doped Electrocatalysts toward Oxygen Evolution Reaction",

abstract = "Introduction of iron in various catalytic systems has served a crucial function to significantly enhance the catalytic activity toward oxygen evolution reaction (OER), but the relationship between material properties and catalysis is still elusive. In this study, by regulating the distinctive geometric sites in spinel, Fe occupies the octahedral sites (Fe3+ (Oh)) and confines Co to the tetrahedral site (Co2+ (Td)), resulting in a strikingly high activity (ηj = 10 mA cm −2 = 229 mV and ηj = 100 mA cm −2 = 281 mV). Further enrichment of Fe ions would occupy the tetrahedral sites to decline the amount of Co2+ (Td) and deteriorate the OER activity. It is also found that similar tafel slope and peak frequency in Bode plot of electrochemical impedance spectroscopy indicate that Co2+ (Td) ions are primarily in charge of water oxidation catalytic center. By means of electrochemical techniques and in situ X-ray absorption spectroscopy, it is proposed that Fe3+ (Oh) ions mainly confine cobalt ions to the tetrahedral site to restrain the multipath transfer of cobalt ions during the dynamic structural transformation between spinel and oxyhydroxide, continuously activating the catalytic behavior of Co2+ (Td) ions. This material-related insight provides an indication for the design of highly efficient OER electrocatalysts.",

keywords = "electrocatalysts, highly efficient, iron, oxygen evolution reaction, water splitting",

author = "Hung, {Sung Fu} and Hsu, {Ying Ya} and Chang, {Chia Jui} and Hsu, {Chia Shuo} and Suen, {Nian Tzu} and Chan, {Ting Shan} and Chen, {Hao Ming}",

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AU - Hung, Sung Fu

AU - Hsu, Ying Ya

AU - Chang, Chia Jui

AU - Hsu, Chia Shuo

AU - Suen, Nian Tzu

AU - Chan, Ting Shan

AU - Chen, Hao Ming

PY - 2018/3/5

Y1 - 2018/3/5

N2 - Introduction of iron in various catalytic systems has served a crucial function to significantly enhance the catalytic activity toward oxygen evolution reaction (OER), but the relationship between material properties and catalysis is still elusive. In this study, by regulating the distinctive geometric sites in spinel, Fe occupies the octahedral sites (Fe3+ (Oh)) and confines Co to the tetrahedral site (Co2+ (Td)), resulting in a strikingly high activity (ηj = 10 mA cm −2 = 229 mV and ηj = 100 mA cm −2 = 281 mV). Further enrichment of Fe ions would occupy the tetrahedral sites to decline the amount of Co2+ (Td) and deteriorate the OER activity. It is also found that similar tafel slope and peak frequency in Bode plot of electrochemical impedance spectroscopy indicate that Co2+ (Td) ions are primarily in charge of water oxidation catalytic center. By means of electrochemical techniques and in situ X-ray absorption spectroscopy, it is proposed that Fe3+ (Oh) ions mainly confine cobalt ions to the tetrahedral site to restrain the multipath transfer of cobalt ions during the dynamic structural transformation between spinel and oxyhydroxide, continuously activating the catalytic behavior of Co2+ (Td) ions. This material-related insight provides an indication for the design of highly efficient OER electrocatalysts.

AB - Introduction of iron in various catalytic systems has served a crucial function to significantly enhance the catalytic activity toward oxygen evolution reaction (OER), but the relationship between material properties and catalysis is still elusive. In this study, by regulating the distinctive geometric sites in spinel, Fe occupies the octahedral sites (Fe3+ (Oh)) and confines Co to the tetrahedral site (Co2+ (Td)), resulting in a strikingly high activity (ηj = 10 mA cm −2 = 229 mV and ηj = 100 mA cm −2 = 281 mV). Further enrichment of Fe ions would occupy the tetrahedral sites to decline the amount of Co2+ (Td) and deteriorate the OER activity. It is also found that similar tafel slope and peak frequency in Bode plot of electrochemical impedance spectroscopy indicate that Co2+ (Td) ions are primarily in charge of water oxidation catalytic center. By means of electrochemical techniques and in situ X-ray absorption spectroscopy, it is proposed that Fe3+ (Oh) ions mainly confine cobalt ions to the tetrahedral site to restrain the multipath transfer of cobalt ions during the dynamic structural transformation between spinel and oxyhydroxide, continuously activating the catalytic behavior of Co2+ (Td) ions. This material-related insight provides an indication for the design of highly efficient OER electrocatalysts.

KW - electrocatalysts

KW - highly efficient

KW - iron

KW - oxygen evolution reaction

KW - water splitting

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Unraveling Geometrical Site Confinement in Highly Efficient Iron-Doped Electrocatalysts toward Oxygen Evolution Reaction

Abstract

Keywords

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