Silicon Anode with High Initial Coulombic Efficiency by Modulated Trifunctional Binder for High‐Areal‐Capacity Lithium‐Ion Batteries

Abstract

storage and engineering heterogeneous structure for lithium transfer are the key for improving the energy density and rate performance of LIBs. [4][5][6][7][8] Silicon (Si), a naturally abundant material with outstanding theoretical capacity (4200 mAh g −1 ), has attracted extensive attention as an alternative promising anode for high-energydensity LIBs, which is ten times larger than the conventional graphite anode (372 mAh g −1 ). [9][10][11][12] However, Si inherently has large volume change that seriously undermines electrode integrity and solid electrolyte interface (SEI) film formed on the Si surface. Repairing and growth of the SEI film leads to reduced amount of available Liions, corresponding to the capacity decline of LIBs. [13][14][15] Generally, engineering Si materials is widely adopted to relieve the influence of large volume change and enhance lithium diffusion within the electrode. [16][17][18] However, high cost is barely accepted into the industry due to complex preparation process. Furthermore, most methods are not based on the mass-loading-oriented strategy for high-energy-density LIBs. [19] Binder is the key component in the electrode to bond active material and conductive additive together on current collector and keep electrode integrity during charge/discharge processes. [20][21][22] Recently, the functions of the binders, such as N-P-LiPN) is constructed by the partially lithiated hard polyacrylic acid as a framework and partially lithiated soft Nafion as a buffer via the hydrogen binding effect. N-P-LiPN has strong adhesion and mechanical properties to accommodate huge volume change of the Si anode. In addition, lithiumions are transferred via the lithiated groups of N-P-LiPN, which significantly enhances the ionic conductivity of the Si anode. Hence, the Si@N-P-LiPN electrodes achieve the highest initial Coulombic efficiency of 93.18% and a stable cycling performance for 500 cycles at 0.2 C. Specially, Si@N-P-LiPN electrodes demonstrate an ultrahigh-areal-capacity of 49.59 mAh cm −2 . This work offers a new approach for inspiring the battery community to explore novel binders for next-generation high-energy-density storage devices. High-capacity electrode materials play a vital role for high-energy-density lithium-ion batteries. Silicon (Si) has been regarded as a promising anode material because of its outstanding theoretical capacity, but it suffers from an inherent volume expansion problem. Binders have demonstrated improvements in the electrochemical performance of Si anodes. Achieving ultrahigh-areal-capacity Si anodes with rational binder strategies remains a significant challenge. Herein, a binder-lithiated strategy is proposed for ultrahigh-areal-capacity Si anodes. A hard/soft modulated trifunctional network binder (

Prelithiation/Presodiation Techniques for Advanced Electrochemical Energy Storage Systems: Concepts, Applications, and Perspectives

“…Considering this characteristic, a binder‐lithiated strategy was proposed for the Si electrode by Li et al ( Figure a). [ 165 ] A hard/soft modulated trifunctional network binder (N‐P‐LiPN) is constructed by the partially lithiated polyacrylic acid (P‐LiPAA) as a framework and partially lithiated Nafion (P‐LiNF) as a buffer via the hydrogen binding effect. The N‐P‐LiPN exhibits strong adhesion and mechanical properties to accommodate huge volume change of the Si anode.…”

“…Reproduced with permission. [ 165 ] Copyright 2020, Wiley‐VCH. b) Schematic of a facile surface coating approach based on a polymeric interphase consisting of polyacrylate salts MPAA (M = Li, Na).…”

“…Expansion of lattice spacing [161] Chemical lithiation N-P-LiNP Amelioration of binder for Si anode [165] Chemical lithiation LiPAA/NaPAA Fabrication of an artificial interphase [166] Chemical lithiation LiPAA SEI layer Decrease of Li dendrite growth [167] Usage of alternatives (SLMP) Graphite Compensation of irreversible capacity loss [92] Usage of alternatives (SLMP) Si-CNT Compensation of irreversible capacity loss [93] Usage of alternatives (Li-Bp-THF) HC Compensation of irreversible capacity loss [97] Usage of alternatives (Li-Bp) SnO 2 /C Compensation of irreversible capacity loss [100] Usage of alternatives (LMNO-R) Si/C and graphite Compensation of irreversible capacity loss [110] Usage of alternatives (Li 3…”

Chemical Coupled PEDOT:PSS/Si Electrode: Suppressed Electrolyte Consumption Enables Long-Term Stability

“…Conventional Si electrodes contain nearly 40 wt% inactive materials, including conductive additive and insulating binders, such as PAA [11], CMC, or alginate [12]. Conducting polymers with dual functions as a binder and conducting additives have been developed for Si anodes [13][14][15][16].…”

Selective Adsorption and Electrocatalysis of Polysulfides through Hexatomic Nickel Clusters Embedded in N-Doped Graphene toward High-Performance Li-S Batteries

“…In imminent pursuit of next-generation electrical energy storage (EES) technologies, lithium-sulfur (Li-S) batteries have attracted enormous research interests due to the high sulfur-specific capacity of 1675 mAh g −1 and the earth-abundant sulfur sources [ 1 – 4 ]. However, the practical application of Li-S batteries is hindered by multiple challenges, i.e., the insulation of S and its discharge products (Li 2 S 2 /Li 2 S), the large volume fluctuation, and the flagrant dissolution of Li 2 S x (4 ≤ x ≤ 8) into the electrolyte during charge/discharge cycles [ 5 ]. One common countermeasure to address the shuttling effects is to adsorb Li polysulfides (LiPSs) through the porous carbon hosts [ 6 ], binder [ 7 ], and membrane [ 8 , 9 ].…”