This study innovatively proposes a“chemical prelithiation/alloying-induced interfacial reconstruction”synergistic strategy that fundamentally improves the performance of Si-based anodes.Through a precisely controlle...This study innovatively proposes a“chemical prelithiation/alloying-induced interfacial reconstruction”synergistic strategy that fundamentally improves the performance of Si-based anodes.Through a precisely controlled process leveraging orbital energetics and Lewis acid catalysis,we successfully engineer a Li-Al-F phase on the interface of SiO(denoted as Pre-SiO-Al)anodes via sequential chemical prelithiation and AlF_(3)-driven interfacial alloying reactions.This novel approach breaks through the ion transport limitations of traditional LiF-dominated solid electrolyte interphase(SEI)layers,while concurrently addressing the critical challenges of low initial Coulombic efficiency(ICE)and severe volume expansion.Mechanism studies reveal that the Li-Al-F offers an ultralow Li^(+)diffusion barrier(0.1 eV),significantly enhancing interfacial ion transport kinetics.Meanwhile,the high mechanical strength and dynamic stress dissipation capability of LiAl-F effectively suppress SEI fracture caused by volume expansion,enabling coordinated deformation compatibility between the electrode and the interfacial layer.The Pre-SiO-Al anode maintains a high capacity of 682.6 m A h g^(-1)after 2000 cycles at 1.0 A g^(-1)with near 100% capacity retention.When paired with LiFePO_(4)cathode,the Pre-SiO-Al||LFP full cell achieves impressive rate capability and cycling stability(93.8% capacity retention after 150 cycles at 0.5 C),demonstrating strong commercialization potential.展开更多
基金the financial support from the National Natural Science Foundation of China(NSFC,No.22308067)the Nature Science Foundation of Guangxi(2025GXNSFBA069166)+2 种基金the Guangxi“Universal Support for Young Talents”Scientific Research Project(ZX02080030424007)the Dean Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology(2022Z009)the Innovation Project of Guangxi Graduate Education(YCSW2024131)。
文摘This study innovatively proposes a“chemical prelithiation/alloying-induced interfacial reconstruction”synergistic strategy that fundamentally improves the performance of Si-based anodes.Through a precisely controlled process leveraging orbital energetics and Lewis acid catalysis,we successfully engineer a Li-Al-F phase on the interface of SiO(denoted as Pre-SiO-Al)anodes via sequential chemical prelithiation and AlF_(3)-driven interfacial alloying reactions.This novel approach breaks through the ion transport limitations of traditional LiF-dominated solid electrolyte interphase(SEI)layers,while concurrently addressing the critical challenges of low initial Coulombic efficiency(ICE)and severe volume expansion.Mechanism studies reveal that the Li-Al-F offers an ultralow Li^(+)diffusion barrier(0.1 eV),significantly enhancing interfacial ion transport kinetics.Meanwhile,the high mechanical strength and dynamic stress dissipation capability of LiAl-F effectively suppress SEI fracture caused by volume expansion,enabling coordinated deformation compatibility between the electrode and the interfacial layer.The Pre-SiO-Al anode maintains a high capacity of 682.6 m A h g^(-1)after 2000 cycles at 1.0 A g^(-1)with near 100% capacity retention.When paired with LiFePO_(4)cathode,the Pre-SiO-Al||LFP full cell achieves impressive rate capability and cycling stability(93.8% capacity retention after 150 cycles at 0.5 C),demonstrating strong commercialization potential.
