Out-of-plane coordination of iridium single atoms with organic molecules and cobalt–iron hydroxides to boost oxygen evolution reaction

Jie Zhao; Yue Guo; Zhiqi Zhang; Xilin Zhang; Qianqian Ji; Hua Zhang; Zhaoqi Song; Dongqing Liu; Jianrong Zeng; Chenghao Chuang; Erhuan Zhang; Yuhao Wang; Guangzhi Hu; Muhammad Asim Mushtaq; Waseem Raza; Xingke Cai; Francesco Ciucci

doi:10.1038/s41565-024-01807-x

Out-of-plane coordination of iridium single atoms with organic molecules and cobalt–iron hydroxides to boost oxygen evolution reaction

Jie Zhao, Yue Guo, Zhiqi Zhang, Xilin Zhang, Qianqian Ji, Hua Zhang, Zhaoqi Song, Dongqing Liu, Jianrong Zeng, Chenghao Chuang, Erhuan Zhang, Yuhao Wang, Guangzhi Hu, Muhammad Asim Mushtaq, Waseem Raza, Xingke Cai^*, Francesco Ciucci^*

^*Corresponding author for this work

School of Energy and Environment

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

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Abstract

Advancements in single-atom-based catalysts are crucial for enhancing oxygen evolution reaction (OER) performance while reducing precious metal usage. A comprehensive understanding of underlying mechanisms will expedite this progress further. Here we report Ir single atoms coordinated out-of-plane with dimethylimidazole (MI) on CoFe hydroxide (Ir₁/(Co,Fe)-OH/MI). This Ir₁/(Co,Fe)-OH/MI catalyst, which was prepared using a simple immersion method, delivers ultralow overpotentials of 179 mV at a current density of 10 mA cm⁻² and 257 mV at 600 mA cm⁻² as well as an ultra-small Tafel slope of 24 mV dec⁻¹. Furthermore, Ir₁/(Co,Fe)-OH/MI has a total mass activity exceeding that of commercial IrO₂ by a factor of 58.4. Ab initio simulations indicate that the coordination of MI leads to electron redistribution around the Ir sites. This causes a positive shift in the d-band centre at adjacent Ir and Co sites, facilitating an optimal energy pathway for OER. © The Author(s) 2024.

Original language	English
Pages (from-to)	57–66
Journal	Nature Nanotechnology
Volume	20
Issue number	1
Online published	21 Oct 2024
DOIs	https://doi.org/10.1038/s41565-024-01807-x
Publication status	Published - Jan 2025

Funding

The work was supported by funding from the National Natural Science Foundation of China (numbers 52003163 and 52373266 received by X.C., number 22105129 received by D.L. and number 22369020 received by J. Zhao), the Guangdong Basic and Applied Basic Research Foundation (numbers 2022A1515010670 and 2024A1515012334 received by X.C. and number 2022A1515011048 received by D.L.), and the Science and Technology Innovation Commission of Shenzhen (numbers KQTD20170810105439418 and 20200812112006001 received by X.C.). The project was funded by the China Postdoctoral Science Foundation (number 2023M732352 received by J. Zhao), and financial support came from the Start-up Research Fund of Southeast University (number RF1028623161 received by Z.Z.) and the Fundamental Research Funds for the Central Universities (number 2242024K40008 received by Z.Z.). We thank the staff of beamline BL13SSW at Shanghai Synchrotron Radiation Facility and the staff at Taiwan Synchrotron Radiation Research Center for XAS experiments support. We also gratefully acknowledge the support of the Research Grant Council of Hong Kong for support through projects 18201820 and 16201622 received by F.C. This work was partly supported by the Project of Hetao Shenzhen-Hong Kong Science and Technology Innovation Cooperation Zone (HZQB-KCZYB-2020083, received by F.C.). F.C. thanks the University of Bayreuth and the Bavarian Center for Battery Technology (BayBatt) for providing a start-up fund. We gratefully acknowledge the valuable assistance of our laboratory colleagues: Y. Li, Y. Wu, Y. Deng, Z. Xie, G. Luo, W. Liu, C. Li, X. Liang, H. Huang, M. Ahmad, L. N. U. Rehman and M. J. Robson. We thank the HKUST Fok Ying Tung Research Institute and National Supercomputing Center in Guangzhou Nansha Sub-Center for providing high-performance computational resources. We also thank H.-Y. Hsu (City University of Hong Kong) and M. Ellwood (The Hong Kong University of Science and Technology) for their support and assistance.

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Zhao, J., Guo, Y., Zhang, Z., Zhang, X., Ji, Q., Zhang, H., Song, Z., Liu, D., Zeng, J., Chuang, C., Zhang, E., Wang, Y., Hu, G., Mushtaq, M. A., Raza, W., Cai, X., & Ciucci, F. (2025). Out-of-plane coordination of iridium single atoms with organic molecules and cobalt–iron hydroxides to boost oxygen evolution reaction. Nature Nanotechnology, 20(1), 57–66. https://doi.org/10.1038/s41565-024-01807-x

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title = "Out-of-plane coordination of iridium single atoms with organic molecules and cobalt–iron hydroxides to boost oxygen evolution reaction",

abstract = "Advancements in single-atom-based catalysts are crucial for enhancing oxygen evolution reaction (OER) performance while reducing precious metal usage. A comprehensive understanding of underlying mechanisms will expedite this progress further. Here we report Ir single atoms coordinated out-of-plane with dimethylimidazole (MI) on CoFe hydroxide (Ir1/(Co,Fe)-OH/MI). This Ir1/(Co,Fe)-OH/MI catalyst, which was prepared using a simple immersion method, delivers ultralow overpotentials of 179 mV at a current density of 10 mA cm−2 and 257 mV at 600 mA cm−2 as well as an ultra-small Tafel slope of 24 mV dec−1. Furthermore, Ir1/(Co,Fe)-OH/MI has a total mass activity exceeding that of commercial IrO2 by a factor of 58.4. Ab initio simulations indicate that the coordination of MI leads to electron redistribution around the Ir sites. This causes a positive shift in the d-band centre at adjacent Ir and Co sites, facilitating an optimal energy pathway for OER. {\textcopyright} The Author(s) 2024.",

author = "Jie Zhao and Yue Guo and Zhiqi Zhang and Xilin Zhang and Qianqian Ji and Hua Zhang and Zhaoqi Song and Dongqing Liu and Jianrong Zeng and Chenghao Chuang and Erhuan Zhang and Yuhao Wang and Guangzhi Hu and Mushtaq, {Muhammad Asim} and Waseem Raza and Xingke Cai and Francesco Ciucci",

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Zhao, J, Guo, Y, Zhang, Z, Zhang, X, Ji, Q, Zhang, H, Song, Z, Liu, D, Zeng, J, Chuang, C, Zhang, E, Wang, Y, Hu, G, Mushtaq, MA, Raza, W, Cai, X & Ciucci, F 2025, 'Out-of-plane coordination of iridium single atoms with organic molecules and cobalt–iron hydroxides to boost oxygen evolution reaction', Nature Nanotechnology, vol. 20, no. 1, pp. 57–66. https://doi.org/10.1038/s41565-024-01807-x

TY - JOUR

T1 - Out-of-plane coordination of iridium single atoms with organic molecules and cobalt–iron hydroxides to boost oxygen evolution reaction

AU - Zhao, Jie

AU - Guo, Yue

AU - Zhang, Zhiqi

AU - Zhang, Xilin

AU - Ji, Qianqian

AU - Zhang, Hua

AU - Song, Zhaoqi

AU - Liu, Dongqing

AU - Zeng, Jianrong

AU - Chuang, Chenghao

AU - Zhang, Erhuan

AU - Wang, Yuhao

AU - Hu, Guangzhi

AU - Mushtaq, Muhammad Asim

AU - Raza, Waseem

AU - Cai, Xingke

AU - Ciucci, Francesco

PY - 2025/1

Y1 - 2025/1

N2 - Advancements in single-atom-based catalysts are crucial for enhancing oxygen evolution reaction (OER) performance while reducing precious metal usage. A comprehensive understanding of underlying mechanisms will expedite this progress further. Here we report Ir single atoms coordinated out-of-plane with dimethylimidazole (MI) on CoFe hydroxide (Ir1/(Co,Fe)-OH/MI). This Ir1/(Co,Fe)-OH/MI catalyst, which was prepared using a simple immersion method, delivers ultralow overpotentials of 179 mV at a current density of 10 mA cm−2 and 257 mV at 600 mA cm−2 as well as an ultra-small Tafel slope of 24 mV dec−1. Furthermore, Ir1/(Co,Fe)-OH/MI has a total mass activity exceeding that of commercial IrO2 by a factor of 58.4. Ab initio simulations indicate that the coordination of MI leads to electron redistribution around the Ir sites. This causes a positive shift in the d-band centre at adjacent Ir and Co sites, facilitating an optimal energy pathway for OER. © The Author(s) 2024.

AB - Advancements in single-atom-based catalysts are crucial for enhancing oxygen evolution reaction (OER) performance while reducing precious metal usage. A comprehensive understanding of underlying mechanisms will expedite this progress further. Here we report Ir single atoms coordinated out-of-plane with dimethylimidazole (MI) on CoFe hydroxide (Ir1/(Co,Fe)-OH/MI). This Ir1/(Co,Fe)-OH/MI catalyst, which was prepared using a simple immersion method, delivers ultralow overpotentials of 179 mV at a current density of 10 mA cm−2 and 257 mV at 600 mA cm−2 as well as an ultra-small Tafel slope of 24 mV dec−1. Furthermore, Ir1/(Co,Fe)-OH/MI has a total mass activity exceeding that of commercial IrO2 by a factor of 58.4. Ab initio simulations indicate that the coordination of MI leads to electron redistribution around the Ir sites. This causes a positive shift in the d-band centre at adjacent Ir and Co sites, facilitating an optimal energy pathway for OER. © The Author(s) 2024.

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JO - Nature Nanotechnology

JF - Nature Nanotechnology

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ER -

Out-of-plane coordination of iridium single atoms with organic molecules and cobalt–iron hydroxides to boost oxygen evolution reaction

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