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MOF-derived XMn 2 O 4 (X = Zn, Co, Cu, Ni) nanomaterials achieve superior electrochemical performance for lithium storage. [Display omitted] • Two methods are proposed for the synthesis of XMn 2 O 4 (X = Zn, Co, Cu, Ni). • MOF-derived anodes exhibit excellent electrochemical capabilities compared with the ones obtained by simple coprecipitation. • Lithium storage capacity and rate performance of XMn 2 O 4 is best when X = Zn. • DFT calculations are performed to demonstrate that ZnMn 2 O 4 as an anode material is conducive to the diffusion of Li+. Bimetallic spinel transition metal oxides play a major part in actualizing eco-friendly electrochemical energy storage systems (ESSs). However, structural precariousness and low electrochemical capacitance restrict their actual implementation in lithium-ion batteries (LIBs). To address these demerits, the sacrificial template approach has been considered as a prospective way to strengthen electrochemical stability and rate performance. Herein, metal-organic frameworks (MOFs) derived XMn 2 O 4 -BDC (H 2 BDC = 1,4-dicarboxybenzene, X = Zn, Co, Cu, Ni) are prepared by a hydrothermal approach in order to discover the effects of various metal cations on the electrochemical performance. Among them, ZnMn 2 O 4 -BDC displays best electrochemical properties (1321.5 mAh g−1 at the current density of 0.1 A g−1 after 300 cycles) and high efficiency with accelerated Li+ diffusivity. Density functional theory (DFT) calculations confirm the ZnMn 2 O 4 possesses the weakest adsorption energy on Li+ with a minimized value of −0.92 eV. In comparison with other XMn 2 O 4 through traditional fabrication method, MOF-derived XMn 2 O 4 -BDC possesses a higher number of Li+ transport channels and better electric conductivity. This tactic provides a feasible and effective method for preparing bimetallic transition metal oxides and enhances energy storage applications. [ABSTRACT FROM AUTHOR]

[Display omitted] • A double-layer coating strategy is used to enhance the performance of SiO x anode. • The dual-shell structure consists of an Sn inner layer and N-doped outer layer. • The inner Sn can improve electronic conductivity and charge transfer kinetics. • The outer N-doped carbon shell can further maintain the structural integrity. • The dual-shell SiO x /C@Sn@NC anode exhibits excellent lithium storage ability. SiO x -based anode materials (0 < x < 2) have been regarded as an appealing candidate for anode material of commercial Lithium-ion batteries accounting for their ultrahigh theoretical capacity and low cost. However, its large-scale applications have been hampered by the serious volume expansion during repeated cycles, low intrinsic conductivity and unsatisfactory initial Coulombic efficiencies. Herein, to address these inherent deficiencies, a hierarchical SiO x -based anode with double-layer coatings of Sn inner layer and N-doped carbon outer shell is elaborately designed by a facile two-step hydrolysis process and polymer coating technology. Benefiting from the "synergistic effect" between Sn and SiO x at different working potentials and a well-designed double-layer coating structure, the resultant SiO x /C@Sn@NC anode displays excellent electrochemical properties, including an enhanced initial Coulomb efficiency (73.3%) efficiency, higher reversible capacity (991 mAh g−1) and superior long lifespan. Moreover, comprehensive characterization based on the reaction kinetics and structural stability proved that such enhanced ICE and cycling stability of anode material stem from its unique double-layer coating structure and multiple active components, which can significantly improve the diffusion of ion and charge transport, stabilize solid-electrolyte interphase (SEI) layer and absorb the expansion stress of electrode. Therefore, this study provides an efficient and feasible strategy to overcome the limitations of high-capacity SiO x -based anode materials via hybridization design with various active components and a double-layer coating strategy. [ABSTRACT FROM AUTHOR]

The hollow Si nanospheres modified by the mechanically robust titanium dioxide (TiO 2 ) shell and the uniform carbon layer are intentionally designed and successfully prepared as the anode active material of high performance lithium-ion batteries. The effects of the robust TiO 2 shell and the uniform carbon layer on the structure and electrochemical performances for the Si@TiO 2 @C nanospheres are studied in detail by X-ray photoelectron spectroscopy, transmission electron microscopy, X-ray diffraction and charge/discharge tests. The results show that the hollow structure of the Si core can spontaneously absorb the huge volume expansion stress, the robust TiO 2 shell is used as a compact fence to promote the expansion towards the interior of the Si cavity instead of the exterior in the processes of charge/discharge, and the uniform carbon layer can effectively enhance the electrical conductivity and further control the integrity and stability of the well-wrapped core-shell-shell framework. Typically, the resultant hollow Si@TiO 2 @C nanospheres exhibit a high initial discharge capacity of 2557.1 mAh g −1 with coulombic efficiency of 86.06% as well as a large recuperative discharge capacity of 1270.3 mAh g −1 after 250 cycles at 1 A g −1 with a mean coulombic efficiency of 99.53%. Therefore, the hollow Si@TiO 2 @C nanospheres prepared by one-step sol-gel coating process show outstanding electrochemical properties and are considered as a prospective candidate to the adhibitions of the anode material for new generation power LIBs. [ABSTRACT FROM AUTHOR]

• Construct carbon protective shell to alleviate huge volume changes of Si. • Robust carbon framework can effectively maintains the structure integrity. • Carbon buffer layer can offer rich e-/ion channels to improve reaction kinetics. • The SCM electrode exhibited excellent electrochemical performance. Si-based anodes have revealed the potential as the next generation of lithium ion battery anode material, whereas the poor conductivity and huge volume changes during (de)lithiation process of silicon still limit their practical application. Herein, the Si/nitrogen doped carbon layer/carbon framework microspheres (SCM) are designed by nano-Si via electro-spray technology as anodes for lithium ion batteries. It has been found that the SCM consists of individual carbon-coated nano-Si primary particles linked by PAN framework, in which the carbon buffer layer can further absorb the stress of volume changes during charge/discharge process, and the carbon framework carbon framework not only provides fast diffusion path of electron, but also effectively reduces the consumption of electrolyte. Therefore, the initial columbic efficiency (ICE) of SCM anode can reach as high as 72%, and the SCM anode also shows a high specific capacity of 1192 mAh g−1 at 0.2 A g−1 and keeps a reversible capacity of 746 mAh g−1 after 200 cycles, demonstrating the as-designed SCM possesses an high ICE and a good electrochemical performance. This strategy provides a significant inspiration for fabricating high-performance Si/C anode materials of lithium-ion battery. [ABSTRACT FROM AUTHOR]