A Multilevel Buffered Binder Network for High-Performance Silicon Anodes

Wan, Xin; Kang, Cong; Mu, Tiansheng; Zhu, Jiaming; Zuo, Pengjian; Yin, Geping

doi:10.1021/acsenergylett.2c02030

Cited by 70 publications

(32 citation statements)

References 40 publications

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“…The local magnification shows this change more clearly (Figure S6). Such results confirm the formation of a hydrogen bond between the silicon particles and c -PAM-CA, which is essential for stabilizing the electrode during charging and discharging. , …”

Section: Resultsmentioning

confidence: 99%

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On-Site Cross-Linking of Polyacrylamide to Efficiently Bind the Silicon Anode of Lithium-Ion Batteries

Liu

Deng

Zhou

et al. 2023

ACS Appl. Mater. Interfaces

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Silicon anode suffers from rapid capacity decay because of its irreversible volume changes during charging and discharging. As one of the important components of the electrode structure, the binder plays an irreplaceable role in buffering the volume changes of the silicon anode and ensuring close contact between various components of the electrode. Traditional PVDF binder is based on weak van der Waals forces and cannot effectively buffer the stress coming from silicon volume expansion, resulting in rapid decay of silicon anode capacity. In addition, most natural polysaccharide binders with a single force face the same problem due to poor toughness. Therefore, it is extremely important to develop a binder with good force and toughness between the silicon particles. Herein, polyacrylamide (PAM) polymer chains that are premixed homogeneously with various components are cross-linked on-site on the current collector via the condensation reaction with citric acid, forming a polar three-dimensional (3D) network with improved tensile properties and adhesion for both silicon particles and current collector. The silicon anode with the cross-linked PAM binder exhibits higher reversible capacity and enhanced long-term cycling stability; the capacity remains at 1280 mA h g–1 after 600 cycles at 2.1 A g–1 and 770.9 mA h g–1 after being subjected to 700 cycles at 4.2 A g–1. It also exhibits excellent cycle stability in silicon–carbon composite materials. This study provides a cost-effective binder engineering strategy, which significantly enhances the long-term cycle performance and stability of silicon anodes, paving the way for large-scale practical applications.

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Section: Resultsmentioning

confidence: 99%

“…Such results confirm the formation of a hydrogen bond between the silicon particles and c-PAM-CA, which is essential for stabilizing the electrode during charging and discharging. 39,40 3.2. Enhanced Mechanical Properties of the On-Site Cross-Linked PAM Binder.…”

Section: Characterization Of the Cross-linking Reaction Between Pam A...mentioning

confidence: 99%

On-Site Cross-Linking of Polyacrylamide to Efficiently Bind the Silicon Anode of Lithium-Ion Batteries

Liu

Deng

Zhou

et al. 2023

ACS Appl. Mater. Interfaces

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“…Figures f and S4 show the electrolyte contact angles of M n + -PODs and PAALi binders. The electrolyte contact angle characterizes the electrolyte wettability of the electrode, which is mainly related to the polar groups of the binders. , Due to the similar SD of M n + -PODs, their electrolyte contact angles are relatively close. Figure f shows that the contact angles of M n + -PODs are around 30°, with minor differences within the margin of error.…”

Section: Resultsmentioning

confidence: 99%

N-Type Polyoxadiazole Conductive Polymer Binders Derived High-Performance Silicon Anodes Enabled by Crosslinking Metal Cations

Sun

Zhu

Yang

et al. 2023

ACS Appl. Mater. Interfaces

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The dilemma of employing high-capacity battery materials and maintaining the electrodes’ electrical and mechanical integrity requires a unique binder system design. Polyoxadiazole (POD) is an n-type conductive polymer with excellent electronic and ionic conductive properties, which has acted as a silicon binder to achieve high specific capacity and rate performance. However, due to its linear structure, it cannot effectively alleviate the enormous volume change of silicon during the process of lithiation/delithiation, resulting in poor cycle stability. This paper systematically studied metal ion (i.e., Li+, Na+, Mg2+, Ca2+, and Sr2+)-crosslinked PODs as silicon anode binders. The results show that the ionic radius and valence state remarkably influence the polymer’s mechanical properties and the electrolyte’s infiltration. Electrochemical methods have thoroughly explored the effects of different ion crosslinks on the ionic and electronic conductivity of POD in the intrinsic and n-doped states. Attributed to the excellent mechanical strength and good elasticity, Ca-POD can better maintain the overall integrity of the electrode structure and conductive network, significantly improving the cycling stability of the silicon anode. The cell with such binders still retains a capacity of 1770.1 mA h g–1 after 100 cycles at 0.2 C, which is ∼285% that of the cell with the PAALi binder (620.6 mA h g–1). This novel strategy using metal-ion crosslinking polymer binders and the unique experimental design provides a new pathway of high-performance binders for next-generation rechargeable batteries.

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“…Functional binders with polar groups (hydroxyl, carboxyl, amino, amide groups, etc. ) − can withstand the volumetric expansion and maintain the overall electrode integrity, because rich hydroxyl groups on the Si surface (Si-OH) can form strong interactions with polar groups by hydrogen bonds or covalent bonds. However, the preparation process of functional binders is usually complicated.…”

Section: Introductionmentioning

confidence: 99%

Prefabrication of “Trinity” Functional Binary Layers on a Silicon Surface to Develop High-Performance Lithium-Ion Batteries

Huang

Wang

et al. 2023

ACS Nano

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The silicon (Si) anode is widely recognized as the most prospective next-generation anode. To promote the application of Si electrodes, it is imperative to address persistent interface side reactions caused by the huge volume expansion of Si particles. Herein, we introduce beneficial groups of the optimized binder and electrolyte on the Si surface by a co-dissolution method, realizing a “trinity” functional layer composed of azodicarbonamide and 4-nitrobenzenesulfonyl fluoride (AN). The “trinity” functional AN interfacial layer induces beneficial reductive decomposition reactions of the electrolyte and forms a hybrid solid–electrolyte interphase (SEI) skin layer with uniformly distributed organic/inorganic components, which can enhance the mechanical strength of the overall electrode, restrain harmful electrolyte depletion reactions, and maintain efficient ion/electron transport. Hence, the optimized Si@AN11 electrode retains 1407.9 mAh g–1 after 500 cycles and still delivers 1773.5 mAh g–1 at 10 C. In stark contrast, Si anodes have almost no reserved capacity at the same test conditions. Besides, the LiNi0.5Co0.2Mn0.3O2//Si@AN11 full-cell maintains 141.2 mAh g–1 after 350 cycles. This work demonstrates the potential of developing multiple composite artificial layers to modulate the SEI properties of various next-generation electrodes.

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A Multilevel Buffered Binder Network for High-Performance Silicon Anodes

Cited by 70 publications

References 40 publications

On-Site Cross-Linking of Polyacrylamide to Efficiently Bind the Silicon Anode of Lithium-Ion Batteries

On-Site Cross-Linking of Polyacrylamide to Efficiently Bind the Silicon Anode of Lithium-Ion Batteries

N-Type Polyoxadiazole Conductive Polymer Binders Derived High-Performance Silicon Anodes Enabled by Crosslinking Metal Cations

Prefabrication of “Trinity” Functional Binary Layers on a Silicon Surface to Develop High-Performance Lithium-Ion Batteries

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