An Anion-Concentrating Layer for a Large-Capacity Al Anode Enabled by an Amorphous 2D Covalent Organic Framework

Juan Li; Wanli Nie; Sergey Ryazantsev; Liping Zhang; Yanan Zhu; Shaohua Guo; Sichen Gu; Chuan Wu

doi:10.1002/adfm.202600038

An Anion-Concentrating Layer for a Large-Capacity Al Anode Enabled by an Amorphous 2D Covalent Organic Framework

Juan Li
, Wanli Nie^*
, Sergey Ryazantsev
, Liping Zhang
, Yanan Zhu
, Shaohua Guo
, Sichen Gu^*
, Chuan Wu^*

^*此作品的通讯作者

Shenzhen MSU-BIT University
Beijing Institute of Technology
Shenzhen Research Institute of HUST

科研成果: 期刊稿件 › 文章 › 同行评审

摘要

Rechargeable aluminum batteries suffer from dendritic anode growth and capacity decay due to severe concentration polarization caused by sluggish ion transport kinetics, particularly under high-capacity conditions. To address this issue, we developed an amorphous covalent organic framework (COF) coating layer engineered for anion-concentrating functionality. The conformational flexible imine linkages in the amorphous COF enable adaptive trapping of Al₂Cl₇⁻, storing them as crystalline AlCl₃ and ligand-bonded AlCl₄⁻ within the mesopores. This mechanism enriches electrochemical active species to buffer the concentration polarization, and promotes the formation of highly active Al₃Cl₁₀⁻ species at the surface, thereby accelerating interfacial kinetics to guide homogeneous deposition. As a result, dendrite-free aluminum deposition is achieved even at an ultrahigh areal capacity of 10 mAh cm⁻² under the protection of the COF. The half-cell with the COF exhibits an exceptional cycling time of over 6000 h with a coulombic efficiency of 99.9%, while symmetric cells demonstrate long-term stability over 7500 h with a low overpotential of 36 mV. Full cells with the graphite cathode also maintain stability over 5000 cycles under a large current density of 1.2 A g⁻¹. This work presents an effective coating strategy for regulating electrodeposition in metal anode batteries, highlighting a promising path toward practical applications.

源语言	英语
文章编号	e00038
期刊	Advanced Functional Materials
卷	36
期	42
DOI	https://doi.org/10.1002/adfm.202600038
出版状态	已出版 - 26 5月 2026
已对外发布	是

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@article{e38d85c465914bf79d32349837da556f,

title = "An Anion-Concentrating Layer for a Large-Capacity Al Anode Enabled by an Amorphous 2D Covalent Organic Framework",

abstract = "Rechargeable aluminum batteries suffer from dendritic anode growth and capacity decay due to severe concentration polarization caused by sluggish ion transport kinetics, particularly under high-capacity conditions. To address this issue, we developed an amorphous covalent organic framework (COF) coating layer engineered for anion-concentrating functionality. The conformational flexible imine linkages in the amorphous COF enable adaptive trapping of Al2Cl7−, storing them as crystalline AlCl3 and ligand-bonded AlCl4− within the mesopores. This mechanism enriches electrochemical active species to buffer the concentration polarization, and promotes the formation of highly active Al3Cl10− species at the surface, thereby accelerating interfacial kinetics to guide homogeneous deposition. As a result, dendrite-free aluminum deposition is achieved even at an ultrahigh areal capacity of 10 mAh cm−2 under the protection of the COF. The half-cell with the COF exhibits an exceptional cycling time of over 6000 h with a coulombic efficiency of 99.9\%, while symmetric cells demonstrate long-term stability over 7500 h with a low overpotential of 36 mV. Full cells with the graphite cathode also maintain stability over 5000 cycles under a large current density of 1.2 A g−1. This work presents an effective coating strategy for regulating electrodeposition in metal anode batteries, highlighting a promising path toward practical applications.",

keywords = "Al anode, aluminum-ion battery, amorphous materials, covalent organic frameworks, large capacity",

author = "Juan Li and Wanli Nie and Sergey Ryazantsev and Liping Zhang and Yanan Zhu and Shaohua Guo and Sichen Gu and Chuan Wu",

note = "Publisher Copyright: {\textcopyright} 2026 Wiley-VCH GmbH.",

year = "2026",

month = may,

day = "26",

doi = "10.1002/adfm.202600038",

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T1 - An Anion-Concentrating Layer for a Large-Capacity Al Anode Enabled by an Amorphous 2D Covalent Organic Framework

AU - Li, Juan

AU - Nie, Wanli

AU - Ryazantsev, Sergey

AU - Zhang, Liping

AU - Zhu, Yanan

AU - Guo, Shaohua

AU - Gu, Sichen

AU - Wu, Chuan

PY - 2026/5/26

Y1 - 2026/5/26

N2 - Rechargeable aluminum batteries suffer from dendritic anode growth and capacity decay due to severe concentration polarization caused by sluggish ion transport kinetics, particularly under high-capacity conditions. To address this issue, we developed an amorphous covalent organic framework (COF) coating layer engineered for anion-concentrating functionality. The conformational flexible imine linkages in the amorphous COF enable adaptive trapping of Al2Cl7−, storing them as crystalline AlCl3 and ligand-bonded AlCl4− within the mesopores. This mechanism enriches electrochemical active species to buffer the concentration polarization, and promotes the formation of highly active Al3Cl10− species at the surface, thereby accelerating interfacial kinetics to guide homogeneous deposition. As a result, dendrite-free aluminum deposition is achieved even at an ultrahigh areal capacity of 10 mAh cm−2 under the protection of the COF. The half-cell with the COF exhibits an exceptional cycling time of over 6000 h with a coulombic efficiency of 99.9%, while symmetric cells demonstrate long-term stability over 7500 h with a low overpotential of 36 mV. Full cells with the graphite cathode also maintain stability over 5000 cycles under a large current density of 1.2 A g−1. This work presents an effective coating strategy for regulating electrodeposition in metal anode batteries, highlighting a promising path toward practical applications.

AB - Rechargeable aluminum batteries suffer from dendritic anode growth and capacity decay due to severe concentration polarization caused by sluggish ion transport kinetics, particularly under high-capacity conditions. To address this issue, we developed an amorphous covalent organic framework (COF) coating layer engineered for anion-concentrating functionality. The conformational flexible imine linkages in the amorphous COF enable adaptive trapping of Al2Cl7−, storing them as crystalline AlCl3 and ligand-bonded AlCl4− within the mesopores. This mechanism enriches electrochemical active species to buffer the concentration polarization, and promotes the formation of highly active Al3Cl10− species at the surface, thereby accelerating interfacial kinetics to guide homogeneous deposition. As a result, dendrite-free aluminum deposition is achieved even at an ultrahigh areal capacity of 10 mAh cm−2 under the protection of the COF. The half-cell with the COF exhibits an exceptional cycling time of over 6000 h with a coulombic efficiency of 99.9%, while symmetric cells demonstrate long-term stability over 7500 h with a low overpotential of 36 mV. Full cells with the graphite cathode also maintain stability over 5000 cycles under a large current density of 1.2 A g−1. This work presents an effective coating strategy for regulating electrodeposition in metal anode batteries, highlighting a promising path toward practical applications.

KW - Al anode

KW - aluminum-ion battery

KW - amorphous materials

KW - covalent organic frameworks

KW - large capacity

UR - https://www.scopus.com/pages/publications/105033034290

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DO - 10.1002/adfm.202600038

M3 - Article

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JO - Advanced Functional Materials

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ER -

An Anion-Concentrating Layer for a Large-Capacity Al Anode Enabled by an Amorphous 2D Covalent Organic Framework

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