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[Display omitted] • Self-assembly by electrostatic interaction between silane and MOF ligand. • The activation mechanism of electrochemical inert metal Co in SiO x materials was investigated. • The catalytic action of atomic Co site activates Si O bond and Li O bond to increase SiO x capacity and coulomb efficiency. • High mechanical strength and high conductivity Co nanoparticles enhance the conductivity and cycling stability of SiO x. The ultra-high theoretical capacity of silicon-based (Si) materials makes them promising anode materials for high energy density lithium-ion batteries. Unfortunately, the dramatic volume change (∼300%) and low electrical conductivity of silicon have severely hindered the commercial use of silicon anodes. Silicon suboxide (SiO x) is one of the ideal candidates for high energy density batteries due to its reduced swelling and lower cost as compared to silicon. However, it remains a huge challenge to address the low conductivity, low (initial) coulombic efficiency and apparent volume effects of SiO x. In this paper, SiO x /Co@C composite anode materials loaded with metal Co nanoparticles were uniformly and efficiently prepared by using 3-aminopropyl triethoxysilane (APTES) as silicon source and Co-MOF as Co source via molecular self-assembly strategy. The experimental results and density functional theory (DFT) calculation showed that the catalytic action of embedded Co nanoparticles had activated the silico-oxygen bond of SiO x and the irreversible product Li 2 O, thereby improving the initial coulombic efficiency (ICE) and enhancing the reversible capacity. At the same time, the metal Co with mechanical rigidity and electrical conductivity alleviated the volume fluctuation during alloying and improved the charge transfer capacity and ion transport rate of the composite. When compared with SiO x @C anodes, SiO x /Co@C-600 composites showed higher initial CE, superior cyclic stability and good rate performance. In particular, the successful matching of the anode with the lithium iron phosphate (LFP) cathode in full cell systems validated the possibility of its practical application. This work provides important insights into the application of Si-based materials in lithium-ion battery electrode materials and the development of high energy density batteries. [ABSTRACT FROM AUTHOR]

SiO x is proposed as one of the most promising high-performance anodes for its favorable capacity and stable lithium insertion/extraction electric potential, however its effective commercial application still faces giant challenge. To overcome poor electrical conductivity and huge volume effect of silicon oxide-based material, we adopt a valid strategy to synthesis the SiO x nanosphere double-wrapped by MoS 2 and multi-walled carbon nanotubes (CNTs) as anode material. The influences of MoS 2 and CNTs on the structure, morphology and electrochemical performances of nanohybrid are probed detailly by transmission electron microscopy, X-ray photoelectron spectroscopy and charge-discharge measurements. The results show that as-prepared nanohybrids release a steady reversible capacity of 798 mAh g−1 with high capacity retention of 81.4% at 500 mA g−1 after 300 cycles. The outstanding electrochemical properties can be ascribed to the facts that the hollow mesoporous structure affords ample buffer space and the introduction of MoS 2 with a two-dimensional layered structure can provide more exposed active-sites for lithium adsorption, as well as the CNTs wrapping can form a favorable conductivity matrix, endowing the nanocomposites with great structural stability. Accordingly, this new structure design by means of a heterogeneous dual-wrapped architecture develops a significant strategy for the development of high-performance SiO x -based anode materials. Unlabelled Image • Heterogeneous dual-wrapped architecture of SiO x /MoS 2 -CNTs is successfully prepared. • The hollow structure shortens the transportation of Li+/e− and offers buffer space. • Wrapping MoS 2 can own more exposed active sites for promoting transport of Li+/e−. • The conductive twining CNTs form a favorable conductivity framework. • The material presents excellent cycling performance and rate capability. [ABSTRACT FROM AUTHOR]