Silicon has attracted ever-increasing attention as a high-capacity anode material in Li-ion batteries owing to its extremely high theoretical capacity. However, practical application of silicon anodes is seriously hindered by its fast capacity fading as a result of huge volume changes during the charge/discharge process. Here, an interpenetrated gel polymer binder for high-performance silicon anodes is created through in-situ crosslinking of water-soluble poly(acrylic acid) (PAA) and polyvinyl alcohol (PVA) precursors. This gel polymer binder with deformable polymer network and strong adhesion on silicon particles can effectively accommodate the large volume change of silicon anodes upon lithiation/delithiation, leading to an excellent cycling stability and high Coulombic efficiency even at high current densities. Moreover, high areal capacity of ∼4.3 mAh/cm2 is achieved based on the silicon anode using the gel PAA–PVA polymer binder with a high mass loading. In view of simplicity in using the water soluble gel polymer binder, it is believed that this novel binder has a great potential to be used for high capacity silicon anodes in next generation Li-ion batteries, as well as for other electrode materials with large volume change during cycling.

Interpenetrated Gel Polymer Binder for High Performance Silicon Anodes in Lithium-Ion Batteries

Energy storage materials are finding increasing applications in our daily lives, for devices such as mobile phones and electric vehicles. Current commercial batteries use flammable liquid electrolytes, which are unsafe, toxic, and environmentally unfriendly with low chemical stability. Recently, solid electrolytes have been extensively studied as alternative electrolytes to address these shortcomings. Herein, we report the early history, synthesis and characterization, mechanical properties, and Li+ ion transport mechanisms of inorganic sulfide and oxide electrolytes. Furthermore, we highlight the importance of the fabrication technology and experimental conditions, such as the effects of pressure and operating parameters, on the electrochemical performance of all-solid-state Li batteries. In particular, we emphasize promising electrolyte systems based on sulfides and argyrodites, such as LiPS5Cl and β-Li3PS4, oxide electrolytes, bare and doped Li7La3Zr2O12 garnet, NASICON-type structures, and perovskite electrolyte materials. Moreover, we discuss the present and future challenges that all-solid-state batteries face for large-scale industrial applications.

Sulfide and Oxide Inorganic Solid Electrolytes for All-Solid-State Li Batteries: A Review

Status and prospect of garnet/polymer solid composite electrolytes for all-solid-state lithium batteries

Advances of polymer binders for silicon-based anodes in high energy density lithium-ion batteries

https://onlinelibrary.wiley.com/doi/pdf/10.1002/sstr.202100009

Challenges and Recent Progress on Silicon-Based Anode Materials for Next-Generation Lithium-Ion Batteries

A conductive self-healing hydrogel binder for high-performance silicon anodes in lithium-ion batteries

A modified natural polysaccharide (carboxymethylated gellan gum) is investigated as a water-soluble high-performance binder for silicon anodes in lithium-ion batteries to improve poor cycle life and fast capacity fade of silicon anodes due to dramatic volume expansion during lithiation/delithiation process. The numberof carboxyl and acetyl groups distributed homogeneously in the modified polysaccharide polymer chain can form strong hydrogen bonds with the surface of Si particle and copper current collector, thus effectively restricting the volume change of silicon and maintaining electronic integrity of Si electrodes during repeated charge/discharge cycles. As a result, Si anodes with carboxymethylated natural polysaccharide polymer present high capacity performance, excellent rate capability, and stable cycling.

A Modified Natural Polysaccharide as a High-Performance Binder for Silicon Anodes in Lithium-Ion Batteries

Ceramic electrolyte guarantees the commercial application of all-solid-state lithium batteries (ASSLBs) for its high ionic conductivity and wide voltage window. However, the large interfacial impedance between the ceramic and polymeric electrolyte is still tough issue for all-solid-state batteries. Here, a "self-sacrifice" interface established by a flexible Li1.5Al0.5Ge1.5(PO4)3 (LAGP)/30% poly(propylene carbonate) (PPC) solid composite electrolyte causes a performance enhancement of the LiFePO4/Li battery with a discharge specific capacity of 151 mA h g-1 at 0.05 C and a retention of 92.3% for 100 cycles at 55 °C without any liquid electrolyte, where the PPC-derived layer swells the Li metal and infiltrates to develop the amorphous state to reduce both interfacial and bulk resistance; while the LAGP with good mechanical strength and the LiF layer provides stability and resists the growth of Li dendrites, which guaranteed the long cycle life and security of batteries. This study demonstrates the complementary advantages of ceramic and polymer, which implies a feasible way to achieve a well-wetted, soft, and stable contact of the electrolyte and electrode to overcome the interface issues in ASSLBs.

Self-Sacrificed Interface-Based on the Flexible Composite Electrolyte for High-Performance All-Solid-State Lithium Batteries.

Silicon (Si) is an auspicious anode material in next-generation lithium-ion batteries due to its exceptional theoretical gravimetric capacity, environmental friendliness, and high natural abundance. However, the practical application of Si anodes remains a "must-solve" challenge because of its drastic capacity fading that results from the inherent property of drastic volume expansion of Si during repeated lithiation and delithiation. Developing binders employed in robust electrodes has been considered an economical and practical method to affect the electrochemical performance of Si-based electrodes. Some natural polymers have demonstrated good adhesive properties with Si-active materials. However, they have limited capacity to keep the structural integrity of electrodes because the network structures solely based on weak hydrogen bonds are susceptible to deformation during cycling. Herein, we develop an in situ covalently cross-linked three-dimensional (3D) supramolecular network and apply it to the Si electrode to improve cycling performance. This network architecture is constructed using furan-modified branched arabinoxylan of corn fiber gum (CFG) and an ionically conductive cross-linker of maleimido-poly(ethylene glycol) (PEG) through the Diels-Alder reaction. The maleimide groups in PEG can react spontaneously with the furan groups in CFG at room temperature without any other stimulation, thus forming strong covalent bonds in the network. The cross-linked CFG-PEG binder has demonstrated robust adhesive properties with Si-active materials and the current collector. The branching of CFG and functional groups of PEG are conducive to improving the lithium-ion conductivity in the silicon anode, resulting in excellent rate performances. The Si anode with a cross-linked CFG-PEG binder exhibits superior cycling stability. As a result, an in situ cross-linking 3D network as a novel binder has a great potential for fabricating an advanced Si anode in next-generation Li-ion batteries.

In Situ Room-Temperature Cross-Linked Highly Branched Biopolymeric Binder Based on the Diels-Alder Reaction for High-Performance Silicon Anodes in Lithium-Ion Batteries.

A lithium ion battery silicon-based negative electrode material aqueous bind and a preparation method and application thereof are provided The commercial food additive gellan gum is subjected to carboxymethylation modification for being applied in the lithium ion battery silicon-based negative electrode material bind Due to the existence of a large number of hydroxyl and carboxyl groups in the molecules, the modified CMGC can form a good adhesion between the silicon material and the current collector, ensure a good electrical contact between the materials, and improve the performance of lithium ion battery; the CMGC binder can dissolve in water easily, and has no pollution to the ecological environment Finally, the raw material of gellan gum of CMGC has been commercialized completely, which significantly reduces the actual industrial production cost and has good market application potential

Shanming Hu

Papers

A conductive self-healing hydrogel binder for high-performance silicon anodes in lithium-ion batteries

A Modified Natural Polysaccharide as a High-Performance Binder for Silicon Anodes in Lithium-Ion Batteries

Self-Sacrificed Interface-Based on the Flexible Composite Electrolyte for High-Performance All-Solid-State Lithium Batteries.

In Situ Room-Temperature Cross-Linked Highly Branched Biopolymeric Binder Based on the Diels-Alder Reaction for High-Performance Silicon Anodes in Lithium-Ion Batteries.

A lithium ion battery silicon-based negative electrode material bind and preparation method and application thereof