Dynamically activating Ni-based catalysts with self-anchored mononuclear Fe for efficient water oxidation

Zhiyuan Zhang; Yuting Luo; Kun Wang; Qiangmin Yu; Xin Kang; Yingqi Liu; Ke Xie; Zhengxing Lv; Zhibo Liu; Fengning Yang; Heming Liu; Ke Liu; Jiong Li; Guangmin Zhou; Wencai Ren; Hui Ming Cheng; Jia Li; Shuo Zhang; Bilu Liu

doi:10.1039/d3ta00866e

Dynamically activating Ni-based catalysts with self-anchored mononuclear Fe for efficient water oxidation

Zhiyuan Zhang, Yuting Luo, Kun Wang, Qiangmin Yu, Xin Kang, Yingqi Liu, Ke Xie, Zhengxing Lv, Zhibo Liu, Fengning Yang, Heming Liu, Ke Liu, Jiong Li, Guangmin Zhou, Wencai Ren, Hui Ming Cheng, Jia Li^*, Shuo Zhang^*, Bilu Liu^*

^*Corresponding author for this work

Chemistry

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

7 Scopus citations

Abstract

Rational design of pre-catalysts to in situ form active structures is vital for efficient catalysis, especially when surface reconstruction occurs. Here we report a surface engineering strategy to form highly active surfaces on Ni-based catalysts (NiMo in this work) under oxygen evolution reaction (OER) conditions. The NiMo catalyst is decorated with mononuclear Fe-O₅ species on its surface. During the OER reconstruction process, the Fe-O₅ species will further bond to the surface of Ni oxyhydroxide reconstructed from NiMo. In situ X-ray absorption spectroscopy and theoretical calculations reveal that the Fe-O₅ species anchored on Ni oxyhydroxide are easily oxidized under OER conditions, which compensates for the charges of Ni and increases the reducibility of Ni active sites. As a result, such a catalyst shows a 33-fold increase in intrinsic activity compared with the NiMo catalyst, which also decreases the full cell voltage by 0.72 V at 500 mA cm⁻² in an anion exchange membrane electrolyzer compared with the IrO₂ catalyst.

Original language	English (US)
Pages (from-to)	10228-10238
Number of pages	11
Journal	Journal of Materials Chemistry A
Volume	11
Issue number	19
DOIs	https://doi.org/10.1039/d3ta00866e
State	Published - Apr 13 2023

Funding

We acknowledge support from the National Science Fund for Distinguished Young Scholars (No. 52125309), National Natural Science Foundation of China (No. 52188101, 11874036, and 11775296), Guangdong Basic and Applied Basic Research Foundation (No. 2021A1515110829 and 2022B1515120004), Guangdong Innovative and Entrepreneurial Research Team Program (No. 2017ZT07C341), Shenzhen Basic Research Project (Nos. JCYJ20200109144620815, JCYJ20200109142816479, WDZC20220812141108001, and WDZC20200819115243002), and the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program (2017BT01N111). We also thank staff at BL11B and BL17U beamlines in the Shanghai Synchrotron Radiation Facility (SSRF) for their technical assistance.

ASJC Scopus subject areas

General Chemistry
Renewable Energy, Sustainability and the Environment
General Materials Science

UN SDGs

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

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10.1039/d3ta00866e

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Zhang, Z., Luo, Y., Wang, K., Yu, Q., Kang, X., Liu, Y., Xie, K., Lv, Z., Liu, Z., Yang, F., Liu, H., Liu, K., Li, J., Zhou, G., Ren, W., Cheng, H. M., Li, J., Zhang, S., & Liu, B. (2023). Dynamically activating Ni-based catalysts with self-anchored mononuclear Fe for efficient water oxidation. Journal of Materials Chemistry A, 11(19), 10228-10238. https://doi.org/10.1039/d3ta00866e

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title = "Dynamically activating Ni-based catalysts with self-anchored mononuclear Fe for efficient water oxidation",

abstract = "Rational design of pre-catalysts to in situ form active structures is vital for efficient catalysis, especially when surface reconstruction occurs. Here we report a surface engineering strategy to form highly active surfaces on Ni-based catalysts (NiMo in this work) under oxygen evolution reaction (OER) conditions. The NiMo catalyst is decorated with mononuclear Fe-O5 species on its surface. During the OER reconstruction process, the Fe-O5 species will further bond to the surface of Ni oxyhydroxide reconstructed from NiMo. In situ X-ray absorption spectroscopy and theoretical calculations reveal that the Fe-O5 species anchored on Ni oxyhydroxide are easily oxidized under OER conditions, which compensates for the charges of Ni and increases the reducibility of Ni active sites. As a result, such a catalyst shows a 33-fold increase in intrinsic activity compared with the NiMo catalyst, which also decreases the full cell voltage by 0.72 V at 500 mA cm−2 in an anion exchange membrane electrolyzer compared with the IrO2 catalyst.",

author = "Zhiyuan Zhang and Yuting Luo and Kun Wang and Qiangmin Yu and Xin Kang and Yingqi Liu and Ke Xie and Zhengxing Lv and Zhibo Liu and Fengning Yang and Heming Liu and Ke Liu and Jiong Li and Guangmin Zhou and Wencai Ren and Cheng, {Hui Ming} and Jia Li and Shuo Zhang and Bilu Liu",

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year = "2023",

month = apr,

day = "13",

doi = "10.1039/d3ta00866e",

language = "English (US)",

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Zhang, Z, Luo, Y, Wang, K, Yu, Q, Kang, X, Liu, Y, Xie, K, Lv, Z, Liu, Z, Yang, F, Liu, H, Liu, K, Li, J, Zhou, G, Ren, W, Cheng, HM, Li, J, Zhang, S & Liu, B 2023, 'Dynamically activating Ni-based catalysts with self-anchored mononuclear Fe for efficient water oxidation', Journal of Materials Chemistry A, vol. 11, no. 19, pp. 10228-10238. https://doi.org/10.1039/d3ta00866e

TY - JOUR

T1 - Dynamically activating Ni-based catalysts with self-anchored mononuclear Fe for efficient water oxidation

AU - Zhang, Zhiyuan

AU - Luo, Yuting

AU - Wang, Kun

AU - Yu, Qiangmin

AU - Kang, Xin

AU - Liu, Yingqi

AU - Xie, Ke

AU - Lv, Zhengxing

AU - Liu, Zhibo

AU - Yang, Fengning

AU - Liu, Heming

AU - Liu, Ke

AU - Li, Jiong

AU - Zhou, Guangmin

AU - Ren, Wencai

AU - Cheng, Hui Ming

AU - Li, Jia

AU - Zhang, Shuo

AU - Liu, Bilu

PY - 2023/4/13

Y1 - 2023/4/13

N2 - Rational design of pre-catalysts to in situ form active structures is vital for efficient catalysis, especially when surface reconstruction occurs. Here we report a surface engineering strategy to form highly active surfaces on Ni-based catalysts (NiMo in this work) under oxygen evolution reaction (OER) conditions. The NiMo catalyst is decorated with mononuclear Fe-O5 species on its surface. During the OER reconstruction process, the Fe-O5 species will further bond to the surface of Ni oxyhydroxide reconstructed from NiMo. In situ X-ray absorption spectroscopy and theoretical calculations reveal that the Fe-O5 species anchored on Ni oxyhydroxide are easily oxidized under OER conditions, which compensates for the charges of Ni and increases the reducibility of Ni active sites. As a result, such a catalyst shows a 33-fold increase in intrinsic activity compared with the NiMo catalyst, which also decreases the full cell voltage by 0.72 V at 500 mA cm−2 in an anion exchange membrane electrolyzer compared with the IrO2 catalyst.

AB - Rational design of pre-catalysts to in situ form active structures is vital for efficient catalysis, especially when surface reconstruction occurs. Here we report a surface engineering strategy to form highly active surfaces on Ni-based catalysts (NiMo in this work) under oxygen evolution reaction (OER) conditions. The NiMo catalyst is decorated with mononuclear Fe-O5 species on its surface. During the OER reconstruction process, the Fe-O5 species will further bond to the surface of Ni oxyhydroxide reconstructed from NiMo. In situ X-ray absorption spectroscopy and theoretical calculations reveal that the Fe-O5 species anchored on Ni oxyhydroxide are easily oxidized under OER conditions, which compensates for the charges of Ni and increases the reducibility of Ni active sites. As a result, such a catalyst shows a 33-fold increase in intrinsic activity compared with the NiMo catalyst, which also decreases the full cell voltage by 0.72 V at 500 mA cm−2 in an anion exchange membrane electrolyzer compared with the IrO2 catalyst.

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JO - Journal of Materials Chemistry A

JF - Journal of Materials Chemistry A

IS - 19

ER -

Dynamically activating Ni-based catalysts with self-anchored mononuclear Fe for efficient water oxidation

Abstract

Funding

ASJC Scopus subject areas

UN SDGs

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