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Nano Research 2024, 17(5): 3919-3926 https://doi.org/10.1007/s12274-023-6388-1
Research Article | Issue | Published: 12 January 2024

Nickel-iron in the second coordination shell boost single-atomic-site iridium catalysts for high-performance urea electrooxidation

Show Author's Information Xiaoyu Chen1,  Jiawei Wan2( ),  Jing Chai3,  Liang Zhang3,  Fang Zhang4,  Qinghua Zhang5,  Lin Gu6,  Lirong Zheng7,  Ranbo Yu1( )
Department of Physical Chemistry, School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing 100083, China
State Key Laboratory of Biochemical Engineering, Key Laboratory of Biopharmaceutical Preparation and Delivery, Chinese Academy of Sciences, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
Center for Combustion Energy, School of Vehicle and Mobility, State Key Laboratory of Intelligent Green Vehicle and Mobility, Tsinghua University, Beijing 100084, China
Analysis and Testing Center, Beijing Institute of Technology, Beijing 100081, China
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
Beijing National Center for Electron Microscopy and Laboratory of Advanced Materials, Department of Materials Science and Engineering, Tsinghua University, Beijing 100084, China
Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
Keywords:
nanoribbon, urea electrooxidation, iridium, single-atom, coordinate structure
Topics:
CatalyticSynthesisEnergy
Cite this article:
Chen X, Wan J, Chai J, et al. Nickel-iron in the second coordination shell boost single-atomic-site iridium catalysts for high-performance urea electrooxidation. Nano Research, 2024, 17(5): 3919-3926. https://doi.org/10.1007/s12274-023-6388-1
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Abstract Full text Electronic supplementary material About this article

Single-atom catalysts (SACs) with high catalytic activity as well as great stability are demonstrating great promotion in electrocatalytic energy conversion, which is also a big challenge to achieve. Herein, we proposed a facile synthetic strategy to construct nickel-iron bimetallic hydroxide nanoribbon stabilized single-atom iridium catalysts (Ir-NiFe-OH), where the nickel-iron hydroxide nanoribbon not only can serve as good electronic conductor, but also can well stabilize and fully expose single-atom sites. Adopted as catalyst for urea oxidation reaction (UOR), it exhibited excellent UOR performance that it only needed a low operated potential of 1.38 V to achieve the current density of 100 mA·cm−2. In-situ Fourier transform infrared spectroscopy, X-ray absorption spectrum, and density functional theory calculations proved that Ir species are active centers and the existence of both Ni and Fe in the local structure of Ir atom can optimize the d-band center of Ir species, promoting the adsorption of intermediates and desorption of products for UOR. The hydrogen evolution reaction (HER)/UOR electrocatalytic cell demanded voltages of 1.46 and 1.50 V to achieve 50 and 100 mA·cm−2, respectively, which demonstrated a higher activity and better stability than those of conventional catalysts. This work opens a new avenue to develop catalysts for UORs with boosted activity and stability.


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Abstract
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Electronic supplementary material
About this article

Nickel-iron in the second coordination shell boost single-atomic-site iridium catalysts for high-performance urea electrooxidation

Show Author's information Xiaoyu Chen1, Jiawei Wan2( ), Jing Chai3, Liang Zhang3, Fang Zhang4, Qinghua Zhang5, Lin Gu6, Lirong Zheng7, Ranbo Yu1( )
Department of Physical Chemistry, School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing 100083, China
State Key Laboratory of Biochemical Engineering, Key Laboratory of Biopharmaceutical Preparation and Delivery, Chinese Academy of Sciences, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
Center for Combustion Energy, School of Vehicle and Mobility, State Key Laboratory of Intelligent Green Vehicle and Mobility, Tsinghua University, Beijing 100084, China
Analysis and Testing Center, Beijing Institute of Technology, Beijing 100081, China
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
Beijing National Center for Electron Microscopy and Laboratory of Advanced Materials, Department of Materials Science and Engineering, Tsinghua University, Beijing 100084, China
Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China

Abstract

Single-atom catalysts (SACs) with high catalytic activity as well as great stability are demonstrating great promotion in electrocatalytic energy conversion, which is also a big challenge to achieve. Herein, we proposed a facile synthetic strategy to construct nickel-iron bimetallic hydroxide nanoribbon stabilized single-atom iridium catalysts (Ir-NiFe-OH), where the nickel-iron hydroxide nanoribbon not only can serve as good electronic conductor, but also can well stabilize and fully expose single-atom sites. Adopted as catalyst for urea oxidation reaction (UOR), it exhibited excellent UOR performance that it only needed a low operated potential of 1.38 V to achieve the current density of 100 mA·cm−2. In-situ Fourier transform infrared spectroscopy, X-ray absorption spectrum, and density functional theory calculations proved that Ir species are active centers and the existence of both Ni and Fe in the local structure of Ir atom can optimize the d-band center of Ir species, promoting the adsorption of intermediates and desorption of products for UOR. The hydrogen evolution reaction (HER)/UOR electrocatalytic cell demanded voltages of 1.46 and 1.50 V to achieve 50 and 100 mA·cm−2, respectively, which demonstrated a higher activity and better stability than those of conventional catalysts. This work opens a new avenue to develop catalysts for UORs with boosted activity and stability.

Keywords: nanoribbon, urea electrooxidation, iridium, single-atom, coordinate structure

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Publication history
Copyright
Acknowledgements

Publication history

Received: 15 October 2023
Revised: 30 November 2023
Accepted: 30 November 2023
Published: 12 January 2024
Issue date: May 2024

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

We acknowledge financial support from the National Natural Science Foundation of China (Nos. 51932001, 51872024, 52022097, and 22293043), the National Key Research and Development Program of China (No. 2018YFA0703503), the Foundation of the Youth Innovation Promotion Association of Chinese Academy of Sciences (No. 2020048). We thank the BL1W1B in BSRF, BL14W1 and BL11B in SSRF for XAS measurement.

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