A Silicon Monoxide Lithium-Ion Battery Anode with Ultrahigh Areal Capacity

Silicon monoxide(SiO)is an attractive anode material for next-generation lithium-ion batteries for its ultra-high theoretical capacity of 2680 mAh g−1.The studies to date have been limited to electrodes with a rela-tively low mass loading(<3.5 mg cm^(−2)),which has seriously restricted the areal capacity and its potential in practical devices.Maximizing areal capacity with such high-capacity materials is critical for capitalizing their potential in practi-cal technologies.Herein,we report a monolithic three-dimensional(3D)large-sheet holey gra-phene framework/SiO(LHGF/SiO)composite for high-mass-loading electrode.By specifically using large-sheet holey graphene building blocks,we construct LHGF with super-elasticity and exceptional mechanical robustness,which is essential for accommodating the large volume change of SiO and ensuring the structure integrity even at ultrahigh mass loading.Additionally,the 3D porous graphene network structure in LHGF ensures excellent electron and ion transport.By systematically tailoring microstructure design,we show the LHGF/SiO anode with a mass loading of 44 mg cm^(−2)delivers a high areal capacity of 35.4 mAh cm^(−2)at a current of 8.8 mA cm^(−2)and retains a capacity of 10.6 mAh cm^(−2)at 17.6 mA cm^(−2),greatly exceeding those of the state-of-the-art commercial or research devices.Furthermore,we show an LHGF/SiO anode with an ultra-high mass loading of 94 mg cm^(−2)delivers an unprecedented areal capacity up to 140.8 mAh cm^(−2).The achievement of such high areal capacities marks a critical step toward realizing the full potential of high-capacity alloy-type electrode materials in practical lithium-ion batteries.

Rational design of F,N-rich artificial interphase via chemical prelithiation initiation strategy enabling high coulombic efficiency and stable micro-sized SiO anodes

Silicon monoxide(SiO)is regarded as a potential candidate for anode materials of lithium-ion batteries(LIBs).Unfortunately,the application of SiO is limited by poor initial Coulombic efficiency(ICE)and unsteady solid electrolyte interface(SEI),which induce low energy,short cycling life,and poor rate properties.To address these drawbacks of SiO,we achieve in-situ construction of robust and fast-ion conducting F,N-rich SEI layer on prelithiated micro-sized SiO(P-μSiO)via the simple and continuous treatment ofμSiO in mild lithium 4,4′-dimethylbiphenyl solution and nonflammable hexafluorocyclotriphosphazene solution.Chemical prelithiation eliminates irreversible capacity through pre-forming inactive lithium silicates.Meanwhile,the symbiotic F,N-rich SEI with good mechanical stability and fast Li^(+)permeability is conductive to relieve volume expansion ofμSiO and boost the Li+diffusion kinetics.Consequently,the P-μSiO realizes an impressive electrochemical performance with an elevated ICE of 99.57%and a capacity retention of 90.67%after 350 cycles.Additionally,the full cell with P-μSiO anode and commercial LiFePO_(4) cathode displays an ICE of 92.03%and a high reversible capacity of 144.97 mA h g^(-1).This work offers a general construction strategy of robust and ionically conductive SEI for advanced LIBs.

Sn Alloy and Graphite Addition to Enhance Initial Coulombic Efficiency and Cycling Stability of SiO Anodes for Li-Ion Batteries

Silicon monoxide(SiO)has aroused increased attention as one of the most promising anodes for high-energy density Li-ion batteries.To enhance the initial Coulombic efficiencies(ICE)and cycle stability of SiO-based anodes,a new facile composition and electrode design strategy have been adapted to fabricate a SiO-Sn-Co/graphite(G)anode.It achieves a unique structure where tiny milled SiO-Sn-Co particles are dispersed among two graphite layers.In this hybrid electrode,Sn-Co alloys promoted Li;extraction kinetics,and the holistic reversibility of SiO and graphite enhanced the electrical conductivity.The SiO-Sn-Co/G electrode delivered an average ICE of 77.6%and a reversible capacity of 640 mAh g^(-1)at 800 mA g^(-1),and the capacity retention was above 98%after 100 cycles,which was much higher than that of the SiO with an ICE of 55.3%and a capacity retention of 50%.These results indicated that this was reliable method to improve the reversibility and cycle ability of the SiO anode.Furthermore,based on its easy and feasible fabrication process,it may provide a suitable choice to combine other alloy anodes with the graphite anode.

Formation mechanisms of Ti_(3)(Si,Al)C_(2)/Al_(2)O_(3) composites from Ti_(3)AlC_(2) and SiO via low-temperature sintering

Ti_(3)SiC_(2)/Al_(2)O_(3) composites have attracted attention due to their excellent mechanical and electromagnetic properties,but the high temperatures(≥1400℃)required for the densification of aluminum oxide(Al_(2)O_(3))leads to the decomposition of Ti_(3)SiC_(2).To address this issue,Ti_(3)(Si_(x)Al_(1−x))C2/Al_(2)O_(3)(x represents the Si content)composites were synthesized for the first time via hot-pressing(HP)sintering and current-assisted sintering(CAS)of mixed Ti_(3)AlC_(2) and silicon monoxide(SiO)powders at 1300 and 1200℃,respectively.Both approaches produced composites with x values greater than 0.9,indicating that the compositions of the prepared composites were similar to those of Ti_(3)SiC_(2)/Al_(2)O_(3) composites.The synthetic mechanism involved substitution and continuous interdiffusion of Al and Si atoms.The composite prepared by CAS at 1200℃ was compacted,whereas the composite prepared by HP had a low density.The low-temperature densification mechanism is attributed to the combined effects of amorphous SiO,liquid Al,and the high heating rates for CAS.The flexural strength and hardness of the composite prepared by CAS were also comparable to those of compacted Ti_(3)SiC_(2)/Al_(2)O_(3) composites.

High-performance SiO/C as anode materials for lithium-ion batteries using commercial SiO and glucose as raw materials

Silicon monoxide(SiO)is considered as a promising anode material for lithium-ion batteries(LIBs)due to its higher capacity and longer cycle life than those of graphite and silicon,respectively.In this study,glucose was developed as a suitable and inexpensive carbon source to synthesize SiO/C composite with a high performance.In addition,the effects of the calcination temperature and the amount of c arbon source on the electrochemical performance of the SiO/C composite were investigated.The addition of 5 wt%glucose and a calcination temperature of 800℃ demonstrated the optimum conditions for SiO/C synthesis.The resultant SiO/C showed an initial charge capacity of 1259 mAh·g^(-1) and a high initial coulombic efficiency of 71.9%.A charge capacity of 850 mAh·g^(-1) after 100 cycles at 200 mA·g^(-1) was achieved,demonstrating the best value of the SiO/C-based materials.The composition changes of SiO under the calcination temperature played a significant role in the electrochemical performance.Overall,the obtained SiO/C material with a high capacity and good stability is suitable for LIB applications as an anode material.

Superior performance for lithium storage from an integrated composite anode consisting of SiO-based active material and current collector

Silicon-based material is considered to be one of the most promising anodes for the next-generation lithium-ion batteries(LIBs)due to its rich sources,nontoxicity,low cost and high theoretical specific capacity.However,it cannot maintain a stable electrode structure during repeated charge/discharge cycles,and therefore long cycling life is difficult to be achieved.To address this problem,herein a simple and efficient method is developed for the fabrication of an integrated composite anode consisting of SiO-based active material and current collector,which exhibits a core-shell structure with nitrogen-doped carbon coating on SiO/P micro-particles.Without binder and conductive agent,the volume expansion of SiO active material in the integrated composite anode is suppressed to prevent its pulverization.At a current density of 500 mA·g−1,this integrated composite anode exhibits a reversible specific capacity of 458 mA·h·g−1 after 200 cycles.Furthermore,superior rate performance and cycling stability are also achieved.This work illustrates a potential method for the fabrication of integrated composite anodes with superior electrochemical properties for high-performance LIBs.