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

Zhao Cai; Daojin Zhou; Maoyu Wang; Seong Min Bak; Yueshen Wu; Zishan Wu; Yang Tian; Xuya Xiong; Yaping Li; Wen Liu; Samira Siahrostami; Yun Kuang; Xiao Qing Yang; Haohong Duan; Zhenxing Feng; Hailiang Wang; Xiaoming Sun

doi:10.1002/anie.201804881

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

Zhao Cai, Daojin Zhou, Maoyu Wang, Seong Min Bak, Yueshen Wu, Zishan Wu, Yang Tian, Xuya Xiong, Yaping Li, Wen Liu, Samira Siahrostami, Yun Kuang, Xiao Qing Yang, Haohong Duan, Zhenxing Feng, Hailiang Wang, Xiaoming Sun

Department of Materials Science and Engineering

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

Abstract

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. Herein 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 cm⁻², which is among the best OER catalytic performance 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. These results reveal the importance of tuning the local atomic structure for designing high efficiency electrocatalysts.

Original language	English
Pages (from-to)	9392-9396
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	57
Issue number	30
DOIs	https://doi.org/10.1002/anie.201804881
Publication status	Published - 2018 Jul 20

Bibliographical note

Funding Information:
This study was supported by the Natural Science Foundation of China, the Program for Changjiang Scholars and Innovative Research Team in the University, and the long-term subsidy mechanism from the Ministry of Finance and the Ministry of Education of P. R. China. The work at Broo-khaven National Laboratory (BNL) was supported by the U.S. Department of Energy, the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies under Contract Number DE-SC0012704. Z.F. thanks the Callahan Faculty Scholar Endowment Fund from Oregon State University. XAS measurements were performed at 9-BM of Advanced Photon Source (APS), Argonne National Laboratory (ANL). The use of APS of ANL is supported by DOE under Contract No. DE-AC02-06CH11357.

Publisher Copyright:
© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

All Science Journal Classification (ASJC) codes

Catalysis
Chemistry(all)

Access to Document

10.1002/anie.201804881

Cite this

Cai, Z., Zhou, D., Wang, M., Bak, S. M., Wu, Y., Wu, Z., Tian, Y., Xiong, X., Li, Y., Liu, W., Siahrostami, S., Kuang, Y., Yang, X. Q., Duan, H., Feng, Z., Wang, H., & Sun, X. (2018). Introducing Fe²⁺ into Nickel–Iron Layered Double Hydroxide: Local Structure Modulated Water Oxidation Activity. Angewandte Chemie - International Edition, 57(30), 9392-9396. https://doi.org/10.1002/anie.201804881

@article{d55876f353864833884e5daeccc13e25,

title = "Introducing Fe2+ into Nickel–Iron Layered Double Hydroxide: Local Structure Modulated Water Oxidation Activity",

abstract = "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. Herein 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 cm−2, which is among the best OER catalytic performance 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. These results reveal the importance of tuning the local atomic structure for designing high efficiency electrocatalysts.",

author = "Zhao Cai and Daojin Zhou and Maoyu Wang and Bak, {Seong Min} and Yueshen Wu and Zishan Wu and Yang Tian and Xuya Xiong and Yaping Li and Wen Liu and Samira Siahrostami and Yun Kuang and Yang, {Xiao Qing} and Haohong Duan and Zhenxing Feng and Hailiang Wang and Xiaoming Sun",

note = "Funding Information: This study was supported by the Natural Science Foundation of China, the Program for Changjiang Scholars and Innovative Research Team in the University, and the long-term subsidy mechanism from the Ministry of Finance and the Ministry of Education of P. R. China. The work at Broo-khaven National Laboratory (BNL) was supported by the U.S. Department of Energy, the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies under Contract Number DE-SC0012704. Z.F. thanks the Callahan Faculty Scholar Endowment Fund from Oregon State University. XAS measurements were performed at 9-BM of Advanced Photon Source (APS), Argonne National Laboratory (ANL). The use of APS of ANL is supported by DOE under Contract No. DE-AC02-06CH11357. Publisher Copyright: {\textcopyright} 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim",

year = "2018",

month = jul,

day = "20",

doi = "10.1002/anie.201804881",

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Cai, Z, Zhou, D, Wang, M, Bak, SM, Wu, Y, Wu, Z, Tian, Y, Xiong, X, Li, Y, Liu, W, Siahrostami, S, Kuang, Y, Yang, XQ, Duan, H, Feng, Z, Wang, H & Sun, X 2018, 'Introducing Fe²⁺ into Nickel–Iron Layered Double Hydroxide: Local Structure Modulated Water Oxidation Activity', Angewandte Chemie - International Edition, vol. 57, no. 30, pp. 9392-9396. https://doi.org/10.1002/anie.201804881

TY - JOUR

T1 - Introducing Fe2+ into Nickel–Iron Layered Double Hydroxide

T2 - Local Structure Modulated Water Oxidation Activity

AU - Cai, Zhao

AU - Zhou, Daojin

AU - Wang, Maoyu

AU - Bak, Seong Min

AU - Wu, Yueshen

AU - Wu, Zishan

AU - Tian, Yang

AU - Xiong, Xuya

AU - Li, Yaping

AU - Liu, Wen

AU - Siahrostami, Samira

AU - Kuang, Yun

AU - Yang, Xiao Qing

AU - Duan, Haohong

AU - Feng, Zhenxing

AU - Wang, Hailiang

AU - Sun, Xiaoming

N1 - Funding Information: This study was supported by the Natural Science Foundation of China, the Program for Changjiang Scholars and Innovative Research Team in the University, and the long-term subsidy mechanism from the Ministry of Finance and the Ministry of Education of P. R. China. The work at Broo-khaven National Laboratory (BNL) was supported by the U.S. Department of Energy, the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies under Contract Number DE-SC0012704. Z.F. thanks the Callahan Faculty Scholar Endowment Fund from Oregon State University. XAS measurements were performed at 9-BM of Advanced Photon Source (APS), Argonne National Laboratory (ANL). The use of APS of ANL is supported by DOE under Contract No. DE-AC02-06CH11357. Publisher Copyright: © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

PY - 2018/7/20

Y1 - 2018/7/20

N2 - 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. Herein 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 cm−2, which is among the best OER catalytic performance 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. These results reveal the importance of tuning the local atomic structure for designing high efficiency electrocatalysts.

AB - 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. Herein 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 cm−2, which is among the best OER catalytic performance 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. These results reveal the importance of tuning the local atomic structure for designing high efficiency electrocatalysts.

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