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

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 w...

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Published inNature nanotechnology Vol. 20; no. 1; pp. 57 - 66
Main Authors Zhao, Jie, Guo, Yue, Zhang, Zhiqi, Zhang, Xilin, Ji, Qianqian, Zhang, Hua, Song, Zhaoqi, Liu, Dongqing, Zeng, Jianrong, Chuang, Chenghao, Zhang, Erhuan, Wang, Yuhao, Hu, Guangzhi, Mushtaq, Muhammad Asim, Raza, Waseem, Cai, Xingke, Ciucci, Francesco
Format Journal Article
LanguageEnglish
Published London Nature Publishing Group UK 01.01.2025
Nature Publishing Group
Subjects
119/118
140/133
140/146
639/301/299/886
639/301/357/1018
639/638/161/886
639/638/77/886
639/925/357/1018
Atomic properties
Catalysts
Chemistry and Materials Science
Cobalt
Coordination
Current density
Evolution
Ferrous hydroxide
Hydroxides
Iridium
Iron
Ligands
Materials Science
Microscopy
Nanoparticles
Nanotechnology
Nanotechnology and Microengineering
Noble metals
Organic chemistry
Oxidation
Oxygen
Oxygen evolution reactions
Precious metals
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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 (Ir 1 /(Co,Fe)-OH/MI). This Ir 1 /(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, Ir 1 /(Co,Fe)-OH/MI has a total mass activity exceeding that of commercial IrO 2 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. This article presents a new method for coordinating iridium atoms with dimethylimidazole and cobalt–iron hydroxides. This enhances the oxygen evolution reaction and delivers high current densities with reduced precious metal use.
AbstractList 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 (Ir 1 /(Co,Fe)-OH/MI). This Ir 1 /(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, Ir 1 /(Co,Fe)-OH/MI has a total mass activity exceeding that of commercial IrO 2 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. This article presents a new method for coordinating iridium atoms with dimethylimidazole and cobalt–iron hydroxides. This enhances the oxygen evolution reaction and delivers high current densities with reduced precious metal use.
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 (Ir /(Co,Fe)-OH/MI). This Ir /(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 and 257 mV at 600 mA cm as well as an ultra-small Tafel slope of 24 mV dec . Furthermore, Ir /(Co,Fe)-OH/MI has a total mass activity exceeding that of commercial IrO 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.
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.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.
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.This article presents a new method for coordinating iridium atoms with dimethylimidazole and cobalt–iron hydroxides. This enhances the oxygen evolution reaction and delivers high current densities with reduced precious metal use.
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 (Ir 1 /(Co,Fe)-OH/MI). This Ir 1 /(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, Ir 1 /(Co,Fe)-OH/MI has a total mass activity exceeding that of commercial IrO 2 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.
Author Cai, Xingke
Mushtaq, Muhammad Asim
Zeng, Jianrong
Guo, Yue
Zhang, Xilin
Zhang, Hua
Hu, Guangzhi
Zhang, Erhuan
Liu, Dongqing
Zhang, Zhiqi
Song, Zhaoqi
Wang, Yuhao
Raza, Waseem
Ji, Qianqian
Chuang, Chenghao
Zhao, Jie
Ciucci, Francesco
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  organization: University of Bayreuth, Chair of Electrode Design for Electrochemical Energy Systems, University of Bayreuth, Bavarian Center for Battery Technology (BayBatt)
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Snippet Advancements in single-atom-based catalysts are crucial for enhancing oxygen evolution reaction (OER) performance while reducing precious metal usage. A...
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StartPage 57
SubjectTerms 119/118
140/133
140/146
639/301/299/886
639/301/357/1018
639/638/161/886
639/638/77/886
639/925/357/1018
Atomic properties
Catalysts
Chemistry and Materials Science
Cobalt
Coordination
Current density
Evolution
Ferrous hydroxide
Hydroxides
Iridium
Iron
Ligands
Materials Science
Microscopy
Nanoparticles
Nanotechnology
Nanotechnology and Microengineering
Noble metals
Organic chemistry
Oxidation
Oxygen
Oxygen evolution reactions
Precious metals
Title Out-of-plane coordination of iridium single atoms with organic molecules and cobalt–iron hydroxides to boost oxygen evolution reaction
URI https://link.springer.com/article/10.1038/s41565-024-01807-x
https://www.ncbi.nlm.nih.gov/pubmed/39433919
https://www.proquest.com/docview/3157760199
https://www.proquest.com/docview/3119190517
https://pubmed.ncbi.nlm.nih.gov/PMC11750697
Volume 20
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