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Gel polymer electrolytes (GPEs) have attracted ever-increasing attention in Li-ion batteries, due to their great thermal stability and excellent electrochemical performance. Here, a flexible poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based GPE doped with an appropriate proportion of the PEO and SiO2 is developed through a universal immersion precipitation method. This porous PVDF-HFP-PEO-SiO2 GPE with high ionic conductivity and lithium-ion transference number (tLi+) can enhance the electrochemical performance of LiFePO4 cells, leading to superior rate capability and excellent cycling stability. Moreover, the PVDF-HFP-PEO-SiO2 GPE effectively inhibits the lithium dendrite growth, thereby improving the safety of Li-ion batteries. In view of the simplicity in using the gel polymer electrolyte, it is believed that this novel GPE can be used as a potential candidate for high-performance Li-ion batteries.

Intercalation transition metal oxides (ITMO) have attracted great attention as lithium-ion battery negative electrodes due to high operation safety, high capacity and rapid ion intercalation. However, the intrinsic low electron conductivity plagues the lifetime and cell performance of the ITMO negative electrode. Here we design a new carbon-emcoating architecture through single CO2 activation treatment as demonstrated by the Nb2O5/C nanohybrid. Triple structure engineering of the carbon-emcoating Nb2O5/C nanohybrid is achieved in terms of porosity, composition, and crystallographic phase. The carbon-embedding Nb2O5/C nanohybrids show superior cycling and rate performance compared with the conventional carbon coating, with reversible capacity of 387?mA?h?g?1 at 0.2?C and 92% of capacity retained after 500 cycles at 1?C. Differential electrochemical mass spectrometry (DEMS) indicates that the carbon emcoated Nb2O5 nanohybrids present less gas evolution than commercial lithium titanate oxide during cycling. The unique carbon-emcoating technique can be universally applied to other ITMO negative electrodes to achieve high electrochemical performance.

Antimony (Sb) has been regarded as one of the most promising anode materials for both lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs) and attracted much attention in recent years. Alleviating the volumetric effect of Sb during charge and discharge processes is the key point to promote Sb-based anodes to practical applications. Carbon dioxide (CO2) activation is applied to improve the rate performance of the Sb/C nanohybrid anodes caused by the limited diffusion of Li/Na ions in excessive carbon components. Based on the reaction between CO2 and carbon, CO2 activation can not only reduce the excess carbon content of the Sb/C nanohybrid but also create abundant mesopores inside the carbon matrix, leading to enhanced rate performance. Additionally, CO2 activation is also a fast and facile method, which is perfectly suitable for the fabrication system we proposed. As a result, after CO2 activation, the average capacity of the Sb/C nanohybrid LIB anode is increased by about 18 times (from 9 mA h g−1 to 160 mA h g−1) at a current density of 3300 mA g−1. Moreover, the application of the CO2-activated Sb/C nanohybrid as a SIB anode is also demonstrated, showing good electrochemical performance.

Niobium dioxide (NbO2) features a high theoretical capacity and an outstanding electron conductivity, which makes it a promising alternative to the commercial graphite negative electrode. However, studies on NbO2 based lithium?ion battery negative electrodes have been rarely reported. In the present work, NbO2 nanoparticles homogeneously embedded in a carbon matrix are synthesized through calcination using a dental resin monomer (bisphenol A glycidyl dimethacrylate, Bis?GMA) as the solvent and a carbon source and niobium ethoxide (NbETO) as the precursor. It is revealed that a low Bis?GMA/NbETO mass ratio (from 1:1 to 1:2) enables the conversion of Nb (V) to Nb (IV) due to increased porosity induced by an alcoholysis reaction between the NbETO and Bis?GMA. The as?prepared NbO2/carbon nanohybrid delivers a reversible capacity of 225 mAh g?1 after 500 cycles at a 1 C rate with a Coulombic efficiency of more than 99.4% in the cycles. Various experimental and theoretical approaches including solid state nuclear magnetic resonance, ex situ X?ray diffraction, differential electrochemical mass spectrometry, and density functional theory are utilized to understand the fundamental lithiation/delithiation mechanisms of the NbO2/carbon nanohybrid. The results suggest that the NbO2/carbon nanohybrid bearing high capacity, long cycle life, and low gas evolution is promising for lithium storage applications.

The cyclability of lithium-ion batteries (LIBs) is often affected by the components of the solid electrolyte interphase (SEI) layer which is generated from electrochemical decomposition of electrolyte. Here, lithium difluorophosphate (LiPO2F2) is studied in this work. When 1.6 wt% LiPO2F2 additive is incorporated into the reference electrolyte, the capacity retention of graphite/Li half-cell is increased from 82.53% to 98.04% and the capacity retention of LiCoO2/Li half-cell is increased from 89.60% to 97.53% after 160 cycles. Electrochemical impedance spectroscopy (EIS) indicates that the SEI layer containing LiPO2F2 can decrease the surface impedance of cells in the last stage cycle. In situ atomic force microscopy (AFM), DFT calculations and X-ray photoelectron spectroscopy (XPS) results show that LiPO2F2 is deposited on the surface of both LiCoO2 and graphite electrodes, which effectively protects the graphite anode and suppresses the degradation of the cathode during the long-term cycling of LIBs.

Electrochemical prelithiation is a facile, effective and extensively used method to improve the initial coulombic efficiency of SiO. However, much less research attention has been devoted to prelithiation effect on initial several cycles. Here, we introduce a new perspective to evaluate the prelithiation behaviors, which could understand in depth the electrochemical prelithiation behaviors and their effects on the following two cycles. Then X-ray photoelectron spectroscopy was further performed to pinpoint the reaction products. It has been found that the quantity of irreversible Li4SiO4, Li2O and SEI (Li2CO3 and LiF) and reversible LixSi are increasing as the prelithiation time extending. When the prelithiation time extending over 20 min, only alloy reaction of Si has been revealed. The regeneration of SEI discloses at least 7% capacity loss in the first cycle which depends on the prelithiated time. However, the reformation of SEI in the second cycles reveals 3% capacity loss. Because the coulombic efficiencies are independent on prelithiated time in the second cycle which indicates only one discharge/charge cycle is enough to form integrated SEI and adequate irreversible Li4SiO4 and Li2O except part of unreactive SiOx.