A Multifunctional Interlocked Binder with Synergistic In Situ Covalent and Hydrogen Bonding for High‐Performance Si Anode in Li‐ion Batteries

Abstract Silicon has garnered significant attention as a promising anode material for high‐energy density Li‐ion batteries. However, Si can be easily pulverized during cycling, which results in the loss of electrical contact and ultimately shortens battery lifetime. Therefore, the Si anode binder is...

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Main Authors: Jae Hyuk Hwang, Eunji Kim, Eun Young Lim, Woohwa Lee, Ji‐Oh Kim, Inhye Choi, Yong Seok Kim, Dong‐Gyun Kim, Jin Hong Lee, Jong‐Chan Lee
Format: Article
Language:English
Published: Wiley 2023-10-01
Series:Advanced Science
Subjects:
Online Access:https://doi.org/10.1002/advs.202302144
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author Jae Hyuk Hwang
Eunji Kim
Eun Young Lim
Woohwa Lee
Ji‐Oh Kim
Inhye Choi
Yong Seok Kim
Dong‐Gyun Kim
Jin Hong Lee
Jong‐Chan Lee
author_facet Jae Hyuk Hwang
Eunji Kim
Eun Young Lim
Woohwa Lee
Ji‐Oh Kim
Inhye Choi
Yong Seok Kim
Dong‐Gyun Kim
Jin Hong Lee
Jong‐Chan Lee
author_sort Jae Hyuk Hwang
collection DOAJ
description Abstract Silicon has garnered significant attention as a promising anode material for high‐energy density Li‐ion batteries. However, Si can be easily pulverized during cycling, which results in the loss of electrical contact and ultimately shortens battery lifetime. Therefore, the Si anode binder is developed to dissipate the enormous mechanical stress of the Si anode with enhanced mechanical properties. However, the interfacial stability between the Si anode binder and Cu current collector should also be improved. Here, a multifunctional thiourea polymer network (TUPN) is proposed as the Si anode binder. The TUPN binder provides the structural integrity of the Si anode with excellent tensile strength and resilience due to the epoxy‐amine and silanol‐epoxy covalent cross‐linking, while exhibiting high extensibility from the random coil chains with the hydrogen bonds of thiourea, oligoether, and isocyanurate moieties. Furthermore, the robust TUPN binder enhances the interfacial stability between the Si anode and current collector by forming a physical interaction. Finally, the facilitated Li‐ion transport and improved electrolyte wettability are realized due to the polar oligoether, thiourea, and isocyanurate moieties, respectively. The concept of this work is to highlight providing directions for the design of polymer binders for next‐generation batteries.
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spelling doaj.art-9e42becc960a4476a8044c94534902f92023-10-26T20:10:11ZengWileyAdvanced Science2198-38442023-10-011030n/an/a10.1002/advs.202302144A Multifunctional Interlocked Binder with Synergistic In Situ Covalent and Hydrogen Bonding for High‐Performance Si Anode in Li‐ion BatteriesJae Hyuk Hwang0Eunji Kim1Eun Young Lim2Woohwa Lee3Ji‐Oh Kim4Inhye Choi5Yong Seok Kim6Dong‐Gyun Kim7Jin Hong Lee8Jong‐Chan Lee9Advanced Materials Division Korea Research Institute of Chemical Technology 141 Gajeong‐ro, Yuseong‐gu Daejeon 34114 Republic of KoreaSchool of Chemical Engineering Pusan National University 2, Busandaehak‐ro 63beon‐gil, Geumjeong‐gu Busan 46421 Republic of KoreaSchool of Chemical Engineering Pusan National University 2, Busandaehak‐ro 63beon‐gil, Geumjeong‐gu Busan 46421 Republic of KoreaAdvanced Materials Division Korea Research Institute of Chemical Technology 141 Gajeong‐ro, Yuseong‐gu Daejeon 34114 Republic of KoreaSchool of Chemical Engineering Pusan National University 2, Busandaehak‐ro 63beon‐gil, Geumjeong‐gu Busan 46421 Republic of KoreaSchool of Chemical Engineering Pusan National University 2, Busandaehak‐ro 63beon‐gil, Geumjeong‐gu Busan 46421 Republic of KoreaAdvanced Materials Division Korea Research Institute of Chemical Technology 141 Gajeong‐ro, Yuseong‐gu Daejeon 34114 Republic of KoreaAdvanced Materials Division Korea Research Institute of Chemical Technology 141 Gajeong‐ro, Yuseong‐gu Daejeon 34114 Republic of KoreaSchool of Chemical Engineering Pusan National University 2, Busandaehak‐ro 63beon‐gil, Geumjeong‐gu Busan 46421 Republic of KoreaSchool of Chemical and Biological Engineering and Institute of Chemical Processes Seoul National University 599 Gwanak‐ro, Gwanak‐gu Seoul 08826 Republic of KoreaAbstract Silicon has garnered significant attention as a promising anode material for high‐energy density Li‐ion batteries. However, Si can be easily pulverized during cycling, which results in the loss of electrical contact and ultimately shortens battery lifetime. Therefore, the Si anode binder is developed to dissipate the enormous mechanical stress of the Si anode with enhanced mechanical properties. However, the interfacial stability between the Si anode binder and Cu current collector should also be improved. Here, a multifunctional thiourea polymer network (TUPN) is proposed as the Si anode binder. The TUPN binder provides the structural integrity of the Si anode with excellent tensile strength and resilience due to the epoxy‐amine and silanol‐epoxy covalent cross‐linking, while exhibiting high extensibility from the random coil chains with the hydrogen bonds of thiourea, oligoether, and isocyanurate moieties. Furthermore, the robust TUPN binder enhances the interfacial stability between the Si anode and current collector by forming a physical interaction. Finally, the facilitated Li‐ion transport and improved electrolyte wettability are realized due to the polar oligoether, thiourea, and isocyanurate moieties, respectively. The concept of this work is to highlight providing directions for the design of polymer binders for next‐generation batteries.https://doi.org/10.1002/advs.202302144in situ cross‐linkingLi‐ion batteriesmultifunctional bindersilicon anodesthiourea polymer network
spellingShingle Jae Hyuk Hwang
Eunji Kim
Eun Young Lim
Woohwa Lee
Ji‐Oh Kim
Inhye Choi
Yong Seok Kim
Dong‐Gyun Kim
Jin Hong Lee
Jong‐Chan Lee
A Multifunctional Interlocked Binder with Synergistic In Situ Covalent and Hydrogen Bonding for High‐Performance Si Anode in Li‐ion Batteries
Advanced Science
in situ cross‐linking
Li‐ion batteries
multifunctional binder
silicon anodes
thiourea polymer network
title A Multifunctional Interlocked Binder with Synergistic In Situ Covalent and Hydrogen Bonding for High‐Performance Si Anode in Li‐ion Batteries
title_full A Multifunctional Interlocked Binder with Synergistic In Situ Covalent and Hydrogen Bonding for High‐Performance Si Anode in Li‐ion Batteries
title_fullStr A Multifunctional Interlocked Binder with Synergistic In Situ Covalent and Hydrogen Bonding for High‐Performance Si Anode in Li‐ion Batteries
title_full_unstemmed A Multifunctional Interlocked Binder with Synergistic In Situ Covalent and Hydrogen Bonding for High‐Performance Si Anode in Li‐ion Batteries
title_short A Multifunctional Interlocked Binder with Synergistic In Situ Covalent and Hydrogen Bonding for High‐Performance Si Anode in Li‐ion Batteries
title_sort multifunctional interlocked binder with synergistic in situ covalent and hydrogen bonding for high performance si anode in li ion batteries
topic in situ cross‐linking
Li‐ion batteries
multifunctional binder
silicon anodes
thiourea polymer network
url https://doi.org/10.1002/advs.202302144
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