Currently, the lithium-ion battery (LIB) is one of the best choices for portable electronic devices and electric vehicles. The energy density of LIBs is only 200-300 Wh kg-1, which is limited by the electrode active materials' capacities. The existing graphite anode, which has low capacity of 372mAh g-1 in commercial LIBs, will need to be replaced in order to reach higher energy densities. Si-based anodes are promising for enhancing the energy density of LIBs because of their high capacity (>4000 mAh g-1), low operating voltages, low cost, and environmental friendliness. However, Si-anodes suffer from large volume expansion (300–400%), thick solid electrolyte interphase (SEI) layer, low conductivity and electrode swelling. For further practical application, it is vital to solve the above issues for improving the performance of Si anodes in LIB. This thesis aims to achieve the above goals by using different organic functionalizing materials to modify the surface of nano Si anode. Firstly, a polymer brush modified core-shell (PBCS) on the Si surface was developed by hydrosilylation reaction. The results indicate that the PBCS structure improves dispersion in slurry, provides mechanical protection during cycling, and enhances electrochemical performance due to intramolecular hydrogen bonding with it and the binder. The Si-PBCS electrode shows the ICE is 87.1%, the retentions are 92.5% (0.1C/ 0.1C) for 200 cycles and 86.2% (0.5C/ 0.5C) for 400 cycles, respectively. Generally, the PBCS structure significantly protects Si from cracking, inhibits gas evolution and non-crystalline formation for improved cycling performance Si anode without FEC additives or carbon coating. Secondly, in-situ polymerization using polymer brush acid and emeraldine base was used to develop a super electrically conductive (SEC) structure on the Si surface for improving the electrochemical stability of Si anode. The results revealed that compared with bare Si electrode, the Si-SEC electrode enhanced electrical conductivity by 104 times, reduced 75% of charge transfer resistance, prevented volume changes with high mechanical properties, and supported high diffusivity of the interfacial layer. The capacity of the Si-SEC electrode remained 1850 mAh g-1 with a 70% retention capacity at 300 cycles without requiring carbon/graphite composites and electrolyte additives. The SEC layer also provides an auto-switch which significantly increases the interfacial impedance to terminate current. Thirdly, an artificial SEI with self-assembled alkyl sulfonic acid (SAASA) structure reinforced is tailored onto the surface of Si through organosilane approach (obtained Si-SAASA anode). A coupling agent, 3-mercaptopropyl trimethoxysilane (MPTMS) was tailored onto the surface of Si producing strong siloxane (Si-O-Si) bond. The thiol group (-SH) in the MPTMS oxidized to sulfonic acid (-SO3H), resulting in a sulfonated artificial SEI reinforcement at the Si surface. With sulfonated MPTMS, the Si anode has been improved by forming -SO3Li, which enhances Li+ diffusion. The Si-SAASA electrode delivers a capacity of 1507.1 mAh g-1 at 0.5 C at 400 cycles with a retention capacity of 74.3%. TThe SAASA structures show good mechanical properties to suppress volume changes, shelters against parasitic reactions, prevent gas evolution, inhibit the formation of thick and high impedance SEI during lithiation/delithiation. A SAASA-based surface modification may extend the life of Si anodes, making the ultimate goal of developing practical LIB based on silicon potential. In conclusion, this thesis developed the need for surface modification of Nano Si to alleviate the causes of large volume change, low electronic conductivity, and instability of SEI layer, which are the key challenges for the performance of Si-based anodes. The study is expected to contribute to the development of a cost effective Si anode for higher-energy LIBs used in electric vehicles.

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