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

Abstract

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.

Biomimetics‐Inspired Architecture Enables the Strength–Toughness of Ultrahigh‐Loading Silicon Electrode

“…As expected, the biomimetic AGO−Si/C electrode, under various mass loading of 1.6, 2.9, 3.5 and 4.1 mg cm −2 , can deliver the impressive areal-capacity of 3.5, 6.9, 7.4, and 10.0 mAh cm −2 , respectively (Figure 4b). It should be noticed that the maximum areal−capacity of biomimetic AGO−Si/C electrode is markedly superior to previous reported Si-based anodes [41][42][43][44][45][46][47][48][49][50][51][52] (Figure 4c; Table S1, Supporting Information). Due to the fast electron/ion migration within 3Dinterweaved carbon architecture, the AGO−Si/C electrode delivers high areal-capacities of 2.2, 2, 1.5, and 1.1 mAh cm −2 under different areal current densities of 0.25, 0.5, 1.25, and 2.5 mA cm −2 , respectively (Figure 4d; Figure S10a, Supporting Information).…”

“…[40] Finally, the progressive cohesion loss of Si particles and cracking of the electrode architecture leads to the rapid capacity decay of LIBs. [41] Therefore, it is critical to break through the inverse relationship between strength and toughness for a very-thick electrode structure. To date, numerous proposals have been studied to maximize the C A − Si .…”

Carbon Nanotube‐Reinforced Dual Carbon Stress‐Buffering for Highly Stable Silicon Anode Material in Lithium‐Ion Battery

“…In the case of bare Si NPs, two peaks at 3478 and 1633 cm −1 correspond to the OH groups on the surface of Si NPs. [ 35 ] After modification with citric acid, the stretching vibration of OH groups for the resulting product (Si@CA) shifts to a lower wavenumber, revealing the formation of a hydrogen bond. [ 36 ] The large negatively charged Si NPs could be well dispersed in the methanol solvent, beneficial for the subsequent ZIF‐67 coating process.…”

Hybrid Ionically Covalently Cross-Linked Network Binder for High-Performance Silicon Anodes in Lithium-Ion Batteries

“…Batteries 2023, 9, x FOR PEER REVIEW 12 cross-linked network ensures the stability of the anode structure, while the reversible ically cross-linked network repeatedly dissipates the mechanical stress generated from lithiation expansion of Si through bond breaking and reconstruction and repairs the d ages to the network structure. The synergy of covalent and ionic bonds enables the hy network binder material to suppress the volume expansion of Si [53] continuously. Figure 8c depicts the variation of the specific capacity of half-cells at current den ranging from 200 to 2000 mA g −1 , enabling an assessment of the impact of CMC-H binders on the rate capacity of Si anodes.…”

“…The covalently cross-linked network ensures the stability of the anode structure, while the reversible ionically cross-linked network repeatedly dissipates the mechanical stress generated from the lithiation expansion of Si through bond breaking and reconstruction and repairs the damages to the network structure. The synergy of covalent and ionic bonds enables the hybrid network binder material to suppress the volume expansion of Si [53] continuously.…”