High-performance Li-ion Batteries Research Articles

Microstructure-Dependent Macroscopic Electro-Chemo- Mechanical Behaviors of Li-Ion Battery Composite Electrodes

The rapid development of the electric vehicle industry has created an urgent need for high-performance Li-ion batteries. Such demand not only requires the development of novel active materials but also requires optimized microstructure of composite electrodes. However, due to complicated heterogeneous electrode microstructure, there still lacks a relationship between the electrode microstructure and the macroscopic electro-chemo-mechanical performance of the battery. In this study, electrochemical and mechanical multi-scale models are developed in order to account for the influence of the heterogeneous microstructure on the macroscopic mechanical and electrochemical behavior of the battery. It is found that porosity and particle size are two important parameters to characterize the microstructure that can affect the macroscopic mechanical and electrochemical behavior. The models developed in this study can be served as designing guidelines for the optimization for the Li-ion battery composite electrodes.

Exploring the potential of carbon and boron nitride integrated biphenyl frameworks as promising anode materials for high-performance Li-ion and Na-ion batteries: A comprehensive first-principles investigation

A protocol of evaluating 2D anode materials that was applied in our previous study has been refined. With the updated Li/Na potential profiles, the two-dimensional biphenyl network (BPN_C) and its isoelectronic structure, boron nitride (BPN_BN), were comprehensively investigated as potential anode materials. The electronic properties, the mechanic strength and the storage capacities were computed accordingly. The band structure results show that the BPN_C and BPN_BN exhibit the nature of conductor and wide-band semi-conductor, respectively. The calculated mechanic strengths of BPN_BN and BPN_C are competent for anode materials. The storage capacities of BPN_C and BPN_BN were addressed by means of the stepwise binding energies (Ead2) and ab initio molecular dynamic simulations. Higher storage capacities were identified as compared with those of the graphene structure. Furthermore, the calculated open-circuit voltages (OCVs) for both BPN_C and BPN_BN can meet the requirements of adequate anode materials. Finally, the diffusivities of Li/Na atoms on the surface of BPN_C and BPN_BN were investigated and found to be suitable for the application as anodes. Our results suggest that the BPN structures can be used as potential anode materials for both LIBs and SIBs.

Hollow core-shell Si-PEI@ZIF-67 with cross-linking effect for high-performance Li-ion batteries

Owing to its extremely high theoretical capacity (4200 mAh g−1), silicon (Si) has emerged as a promising candidate for lithium-ion batteries (LIBs) anodes. However, challenges such as a volumetric expansion of up to 300 % and poor electrical conductivity have impeded its application. Here, hollow core-shell Si-PEI@ZIF-67 synthesized via a simple one-pot method utilizing the unique properties of ZIF-67, including its porous nature, high surface area, and well-ordered structure, ZIF-67 coating effectively mitigates the volume expansion of nano-Si during cycles. Hollow core-shell structure can accelerate ion transfer and alleviate volume expansion. Moreover, Co2+ enrichment in the coating promotes the formation of a strong cross-linking network with the binder sodium alginate. This interaction not only enhances the adhesion between active material and current collector but also accelerates ion transport. Si-PEI@ZIF-67 composites demonstrate outstanding lithium storage performance in LIBs, achieving a stable capacity of 1134.4 mAh g−1 after 500 cycles at 1000 mA g−1. In addition, the discharge capacity of 828.7 mAh g−1 is maintained after 200 cycles at the high current density of 5000 mA g−1. The innovative synthesis method, utilizing ZIF-67 as a coating for nano-Si and establishing an interconnected network with the binder, offers a novel approach for other anodes.

Effect of strontium phosphate coating on NCM811 powders for high-performance Li-ion battery cathode

The NCM811 cathode material, characterized by a high nickel content, is known for its substantial energy capacity but is afflicted by challenges, including electrolyte degradation and inadequate cyclic stability. In this study, a chemical bath deposition technique is utilized to apply a layer of Sr3(PO4)2 material onto the surface of NCM811 particles to address these problems. This procedure yields a continuous protective coating that shields the NCM811 particles from detrimental interactions with the electrolyte, such as HF attack and the formation of surface cracks, while also promoting the diffusion of lithium ions during charge/discharge cycles. XRD analysis indicated that the application of Sr3(PO4)2 coating did not cause any changes in the structure of the NCM811 cathode material. SEM images of all coated samples demonstrated that all coated samples have spherical morphology. Additionally, both Raman and FTIR examinations provide evidences supporting the existence of strontium phosphate material on the surface of the NCM811 cathode material. The distinctive 5.9 nm-thick Sr3(PO4)2 coating enables the NCM811 material to maintain 96 % of its capacity after 100 charge/discharge cycles in a voltage range of 2.8–4.4 V vs. Li/Li+ at a current rate of 1C.

High-performance Li-ion battery cathode: Mn-doped LiFePO4 via solution combustion synthesis method

The main drawbacks of LiFePO4, namely low electronic conductivity and slow lithium ion diffusion, are overcome by doping through solution combustion synthesis. This study focuses on altering the properties of LiFePO4 cathode material by introducing manganese (Mn) into the Fe site. Using solution combustion synthesis, we successfully created Mn-doped LiFe1-xMnxPO4 samples (where x = 0.04, 0.08, and 0.12) as it provides highly pure and crystalline material with homogeneous incorporation of dopants. Through various analyses including X-ray diffraction (XRD), RAMAN spectroscopy, scanning electron microscopy (SEM), transmission electron microscopy (TEM), EDAX, X-ray photoelectron spectroscopy (XPS), BET surface area measurement, charge/discharge tests (CD), stability assessments, and rate performance evaluations, we uncovered insights into the structure, morphology, elemental composition, surface area, and electrochemical properties of the synthesized materials. Notably, the LiFe0.92Mn0.08PO4 sample exhibited an average capacity of 166.34 mAh/g over 100 cycles at a 0.1C rate, slightly below its theoretical capacity of 170 mAh/g.

Exploring the Nb-Ti-W-O System for Use as Li-Ion Battery Anodes

While much attention in recent years has been given to high performance Li-ion batteries for electrical vehicles, other applications such as medical devices require a unique set of properties that demand a different set of material considerations such as long lifetimes and extremely high safety. Anodes for such batteries must be carefully selected to properly achieve these goals. The most commonly industrially utilized anode material, graphite, is not suitable for medical applications due to particle fracture and Li dendrite growth at high rates. Currently utilized medical device anode materials obtain this high performance by sacrificing energy density.Herein a new set of Nb based materials for use as anodes are presented that do not need to make such a sacrifice as they display high longevity along with high energy densities. The Nb-Ti-W pseudoternary features many promising single-phase compositions that could be used as anodes for such devices. These compositions derive from crystal structures that are found on both the Nb2O5-WO3 and Nb2O5-TiO2 pseudobinaries1, though they posses a more diverse range of chemical compositions. These compositions feature high performance discharge capacities of up to 300 mAh/g. Some materials also display robust capacity retentions of up to 98% after 10 cycles. The materials were also tested at 37 °C to simulate operation within the human body. At these temperatures, improvements were found in electrochemical performance for nearly all compositions, notably demonstrating a large improvement in capacity retention regardless of crystal structure. References (1) Rehman, S.; Sieffert, J. M.; Lang, C. J.; McCalla, E. NbyW1-yOz and NbxTi1-xOz pseudobinaries as anodes for Li-ion batteries. Electrochimica Acta 2023, 439. DOI: 10.1016/j.electacta.2022.141665.

Why Charge Rate Capability Tests Fail to Characterize Structured Electrodes in Lithium-Ion Batteries and How to Modify Them

Fast charging is one of the most essential criteria for the user acceptance of battery electric vehicles. Especially for high-loaded electrodes used in automotive applications, the rate capability is limited due to the transport limitations of lithium ions in the pores.1 Electrode structuring is a powerful tool to overcome those limitations by creating additional directed diffusion channels for lithium ions.2 Despite the frequently described reduction of the transport limitation of lithium-ion batteries,3 there are hardly any charge rate capability tests in the literature that demonstrate the improvement through structuring. Instead, most studies present discharge rate capability tests showing the desired performance increase due to structuring.4-8 This study will explain why charge rate capability tests fail to characterize electrodes in the transport-limiting C-rate range. For this purpose, graphite anodes underwent “structure calendering”, where electrodes are simultaneously mechanically structured and calendered using an embossing roller. Thus, identical electrode properties, except for the lower tortuosity, can be achieved compared to the non-structured graphite anodes that were only calendered. Despite their different tortuosities, we will show that structured and non-structured graphite anodes exhibit minimal capacity differences in the charge rate capability test. This is attributed to lithium plating, which shifts the anode potential to similar values, regardless of the transport properties of the investigated electrode. We will modify the test to characterize the charge rate capability of electrodes in the transport-limiting regime where lithium plating occurs. For this purpose, in the charge rate capability test, the current is superimposed with a sinusoidal signal and the voltage response is measured. This allows the continuous estimation of the cell impedance during charging. Previous studies have shown that this method allows to track the onset of the lithium plating reaction.9-10 Applying the modified charge rate capability test will demonstrate that this detrimental side reaction occurs significantly later in structured electrodes. Günter, F. J., & Wassiliadis, N. (2022). State of the Art of Lithium-Ion Pouch Cells in Automotive Applications: Cell Teardown and Characterization. Journal of The Electrochemical Society, 169(3), 030515. https://doi.org/10.1149/1945-7111/ac4e11Pfleging, W. (2017). A review of laser electrode processing for development and manufacturing of lithium-ion batteries. Nanophotonics, 7(3), 549–573. https://doi.org/10.1515/nanoph-2017-0044Mai, W., Usseglio-Viretta, F. L. E., Colclasure, A. M., & Smith, K. (2020). Enabling fast charging of lithium-ion batteries through secondary-/dual- pore network: Part II - numerical model. Electrochimica Acta, 341, 136013. https://doi.org/10.1016/j.electacta.2020.136013Keilhofer, J., Schaffranka, L., Wuttke, A., Günter, F., Hille, L., Dorau, F., & Daub, R. (2023). Mechanical Structuring of Lithium‐Ion Battery Electrodes Using an Embossing Roller. Energy Technology. https://doi.org/10.1002/ente.202200869Dubey, R., Zwahlen, M. D., Shynkarenko, Y., Yakunin, S., Fuerst, A., Kovalenko, M. V., & Kravchyk, K. V. (2021). Laser Patterning of High-Mass-Loading Graphite Anodes for High-Performance Li-Ion Batteries. Batteries and Supercaps, 4(3), 464–468. https://doi.org/10.1002/batt.202000253Habedank, J. B., Kriegler, J., & Zaeh, M. F. (2019). Enhanced Fast Charging and Reduced Lithium-Plating by Laser-Structured Anodes for Lithium-Ion Batteries. Journal of The Electrochemical Society, 166(16), A3940–A3949. https://doi.org/10.1149/2.1241915jesHabedank, J. B., Kraft, L., Rheinfeld, A., Krezdorn, C., Jossen, A., & Zaeh, M. F. (2018). Increasing the Discharge Rate Capability of Lithium-Ion Cells with Laser-Structured Graphite Anodes: Modeling and Simulation. Journal of The Electrochemical Society, 165(7), A1563–A1573. https://doi.org/10.1149/2.1181807jesHille, L., Xu, L., Keilhofer, J., Stock, S., Kriegler, J., & Zaeh, M. F. (2021). Laser structuring of graphite anodes and NMC cathodes – Proportionate influence on electrode characteristics and cell performance. Electrochimica Acta, 392, 139002. https://doi.org/10.1016/j.electacta.2021.139002Koseoglou, M., Tsioumas, E., Ferentinou, D., Jabbour, N., Papagiannis, D., & Mademlis, C. (2021). Lithium plating detection using dynamic electrochemical impedance spectroscopy in lithium-ion batteries. Journal of Power Sources, 512(September), 230508. https://doi.org/10.1016/j.jpowsour.2021.230508Straßer, A., Adam, A., & Li, J. (2023). In operando detection of Lithium plating via electrochemical impedance spectroscopy for automotive batteries. Journal of Power Sources, 580(July), 233366. https://doi.org/10.1016/j.jpowsour.2023.233366

A novel multifunctional electrolyte system for high performance Li-ion batteries

Lithium-ion batteries have advantages such as environmental protection and sustainable use, but the widespread application of lithium-ion battery-powered vehicles is limited by the inability to quickly charge and extreme ambient temperatures, and reasonable design of electrolyte components can effectively solve these problems. Here, a novel fluoroethylene carbonate (FEC)/ethyl acetate (EA) based electrolyte containing lithium difluorophosphate (LiPO2F2, 2 wt%) and lithium bis(fluorosulfonyl)imide salt (LiFSI, 1.0 M) is first reported. The electrolyte containing these components has the characteristics of low freezing point, low viscosity and high ionic conductivity. Especially, due to the preferential decomposition of FEC, LiFSI and LiPO2F2, uniform multiphase inorganic LiF and Li3N species are formed on the electrode surface with enhanced robustness and ion transfer kinetics. So, the graphite||LiNi0.5Co0.2Mn0.3O2&LiMn2O4 (Gr||LMO&NCM523) batteries in the designed electrolyte maintain high capacity and coulombic efficiency (100 %) after 200 times at 1C charge and discharge current density at 25 °C and 45 °C. At −20 °C, the batteries have a coulombic efficiency of 50 % and capacity of 38.0 mA h g−1 after 200 charging and discharging cycles, showing excellent low-temperature fast dynamics. Our work supplies an efficient way to accelerate the engineering application of Li-ion batteries.

Facile synthesis of novel bismuth oxide/bismuth molybdate nanocomposites as advanced anodes for high performance Li‐ion batteries

In this study, a novel nanocomposite material consisting of Bi2O3 and Bi2MoO6, named as Bi2O3@Bi2MoO6, was successfully fabricated by co-precipitation method in ethylene glycol solvent. Morphological analysis of the heat-treated sample at 400 oC for 12 h in Ar atmosphere (Bi2O3@Bi2MoO6 _400oC) showed that it contained nano-sized particles of Bi2O3 and Bi2MoO6; in addition, an amorphous phase along with a crystalline structure was also observed. When used as an anode for Li-ion batteries (LIBs), Bi2O3@Bi2MoO6 _400oC anode exhibits excellent electrochemical properties such as high Coulombic efficiency, high specific capacity, excellent capacity retention, and outstanding rate capacity. Specifically, the Bi2O3@Bi2MoO6 _400oC anode presented a reversible capacity of 786 mAh g-1 at the beginning cycle at 0.1 A g-1 and retained about 90% of the charging capacity value after 80 cycles. The advanced electrochemical properties of the nanocomposite anode are related to the combination of many aspects such as nanostructure, existence of amorphous phase, and pseudo-behaviour of metal-based components. The structural stability and electrochemical performance of the anode material, therefore, are improved. These results demonstrate Bi2O3@Bi2MoO6 _400oC as a promising material for establishing high-performance LIB anodes.

Study on the role of d electronic donor in Ni-rich layered oxide cathode materials for Li-ion battery

The further development of electrochemical devices and electric vehicles requires advanced Li-ion battery with higher energy density and longer lifetimes. Ni-rich LiNi0.8Co0.1Mn0.1O2 layered oxide cathodes are receiving increased attention due to its high specific capacity. Nevertheless, the role of d electrons in Ni-rich cathodes has not been uniformly reported, which hinders the design of high-performance Ni-rich cathodes. To address this issue, the role of d electronic donor in Ni-rich layered oxide cathode materials was investigated by first principles calculations and explored the mechanism for enhancing the electrochemical performance in this work. The results show that the d electronic donor V and Mo can elevate the intercalation potential, improve the stability, and enhance the diffusion rate of Li-ions in Ni-rich cathode. This theoretical study complements the mechanism for improving the electrochemical performance of Ni-rich cathode, and provides a theoretical basis for the design of high-performance Li-ion battery.

Ultrathin composite Al2O3/LiAlO2 coating on truncated octahedral shape Co-free LiNi0.5Mn1.5O4 for enable high performance Li-ion battery

The Co-free cathode material of spinel LiNi0.5Mn1.5O4 (LNMO) has gained much interest for next-generation batteries owing to its 3D ionic channel for fast Li+ ion diffusion and high voltage operation. In this work, ultrathin composite Al2O3/LiAlO2 is adopted to modify truncated octahedral shape Fd3¯m spinel LNMO. It is found that 1 wt% Al coating modification exhibits the most excellent cycling performances, providing great capacity retention of 84.99 % for 350 cycles between 3.5 and 4.8 V at 1C. The homogeneous composite Al2O3/LiAlO2 coating on the truncated octahedral shape particle can deliver high rate capability of 40 mAh/g at 20C, charging and discharging. In addition, the ultrathin composite Al2O3/LiAlO2 coating can provide a stable interface, producing a high capacity retention of 94.82 % after 100 cycles at 45 °C. High performances of truncated octahedral shape Fd3¯m LNMO by composite Al2O3/LiAlO2 coating can enhance the safety and increase the potential applications of these cathode materials in the next-generation batteries.

A like-bulletproof glass structure flexibility-rigidity coating layer strategy for high-performance Li ion batteries Si anodes

In order to overcome the problems about the volume expansion and poor electronic conductivity of Si, a flexibility and rigidity double coating layer CNTs-rGO- PAIN was constructed. The CNTs-rGO-PANI network with porous structure and high electronic conductivity provides sufficient space to accommodate the volume change of Si, and abundant transmission path for electron and Li ion. Moreover, the coating network with flexibility and rigidity characteristic could absorb the expansion stress of Si, maintain electrode structural integrity, promote the growth of stable SEI. The polymer-nanocarbon network dual coating layer effectively safeguards the electrochemical-mechanical interplay within the electrode. The 20Si-CNTs-rGO-PANI exhibits a reversible capacity as high as 1856 mAh g−1 after 400 cycles at 0.2 A g−1 and a remarkable rate capacity of 570 and 459 mAh g−1, at 5 and 10 A g−1, respectively. The outstanding Li ion storage performance of 20Si-CNTs-rGO-PANI anode, suggests the flexibility-rigidity dual coating layer strategy is a potential way to improve the performance of alloy type anode.

Electrospun Co-Ni mixed multiple oxidation states heterostructure for high-performance Li-ion battery

With the increasing prevalence of mobile electronic devices, electric vehicles, and other technological advancements, there is a growing demand for higher-capacity Lithium-ion batteries (LIBs). Metal-organic frameworks (MOFs) have been actively researched in recent years due to their numerous advantages. However, the irreversible collapse during lithium-ion interaction hampers MOFs’ electrochemical stability. This study employs a direct precipitation method to synthesize uniformly shaped MOF materials, followed by carbon coating using electrospinning techniques, and ultimately, derivatives of MOF materials are produced through annealing. Thanks to this innovative material design process, exceptional performance is observed in this material as a lithium-negative electrode. After 1000 cycles at a high current density of 1 A g−1, its reversible capacity stabilizes at 1318 mAh g−1. Moreover, this negative electrode material exhibits exceptional rate performance at various current densities. The Co3O4/NiO@NCNFs electrode demonstrates enhanced charge storage capacity due to the synergistic effects of diffusion and capacitance control processes. Additionally, this material exhibits characteristics of low impedance and high lithium-ion diffusion rate. This study presents a novel method for manufacturing lithium-ion battery negative electrode materials by integrating MOF materials with electrospinning technology.

3D-printed topological-structured electrodes with exceptional mechanical properties for high-performance flexible Li-ion batteries

A vital aspect in advancing flexible batteries is the development of flexible electrodes capable of enduring repeated stretching while upholding satisfactory electrochemical performance. Thus, adopting a systematic and efficient approach to structural design and fabrication becomes imperative. In this study, we introduce an optimal structural design achieved through topology optimization and fabricate flexible electrodes via 3D printing, representing a departure from traditional design and manufacture methodologies in the development of flexible electrodes for batteries. Our research underscores the impressive mechanical strength of these topologically-structured electrodes (TSEs), validated through rigorous finite element analysis (FEA) and tensile strength testing. The results of both the stretch deformation and twist deformation analysis on the TSEs and the conventional mesh-structured electrodes (MSEs) show that the peak strain and stress of TSEs are much lower than those of MSEs. Notably, even under 50 % stretching, the TSEs maintain structural integrity, contrasting sharply with conventional mesh-structured electrodes (MSEs) and flat film electrodes which often crack under similar conditions. Moreover, after enduring 50 cycles of stretching, the TSEs retain an outstanding 98 % of their original capacity, surpassing MSEs which retain only 80 % of their capacity. These findings highlight the significant potential of topologically designed flexible electrodes, offering promising avenues for the development of stretchable and flexible energy storage devices such as wearable tech and bio-integrated electronics.

Electrolyte Design Chart Reframed by Intermolecular Interactions for High-Performance Li-Ion Batteries.

Developing advanced electrolytes has been regarded as a pivotal strategy for enhancing the electrochemical performance of batteries; however, the criteria for electrolyte design remain elusive. In this study, we present an electrolyte design chart reframed through intermolecular interactions. By combining systematic nuclear magnetic resonance, Fourier transform infrared measurements, molecular dynamics (MD) simulations, and machine-learning-assisted classifications, we establish semiquantitative correlations between electrolyte components and the electrochemical reversibility of electrolytes. We propose the equivalent increment of Li salt resulting from functional cosolvent and solvent-solvent interactions for effective electrolyte design and prediction. The controllable regulation of the electrolyte design chart by the properties of solvent-solvent interactions presents varying equivalent effects of increasing Li salt concentrations in different electrolyte systems. Based on this mechanism, we demonstrate highly reversible and nonflammable phosphate-based electrolytes for graphite||NCM811 full cells. The proposed electrolyte design chart, semiquantitatively determined by intermolecular interactions, provides the necessary experimental foundation and basis for the future rapid screening and prediction of electrolytes using machine-learning methods.

Well-dispersed Sb particles embedded on N-doped carbon nanofibers toward high-performance Li-ion battery

Well-dispersed Sb particles embedded on N-doped carbon nanofibers toward high-performance Li-ion battery

Unlocking the power of lithium trifluoride, LiMF3 (M = Mn, Co, Fe, Ni, and V), materials through DFT: a paradigm shift in electrode candidates for high-performance Li-ion batteries

Unlocking the power of lithium trifluoride, LiMF3 (M = Mn, Co, Fe, Ni, and V), materials through DFT: a paradigm shift in electrode candidates for high-performance Li-ion batteries

Synergistic construction of uniform LiAlO2 coating on LiNi0.8Co0.1Mn0.1O2 cathode materials by acid etching and polyvinylpyrrolidone cross-linking approaches for high-performance Li-ion batteries

A uniform and conductive LiAlO2 coating on the LiNi0.8Co0.1Mn0.1O2 cathode material was successfully constructed by the synergistic effects of acid etching and polyvinylpyrrolidone (PVP) cross-linking approaches. Hydrolysis of Al sources (Al(NO3)3) generates H+ ions to etch the inert surfaces of hydroxide precursors, which leaves highly active sites exposed on the Ni0.8Co0.1Mn0.1(OH)2 surfaces for subsequent coating. Furthermore, PVP polymeric chains act as cross-linkers to anchor Al(OH)3 onto the highly active Ni0.8Co0.1Mn0.1(OH)2 surfaces for the formation of uniform LiAlO2 coating layers after chemical lithiation of calcination. The synergistically constructed LiAlO2 coating layers could effectively reduce the gas production and improve the cycling stability of the LiNi0.8Co0.1Mn0.1O2 cathode materials with a high reversible capacity of 212.0 mAh g−1 at 0.1 C for the initial cycle and 172.3 mAh g−1 at 1 C for the 200th cycle.

A Macromolecule Cathode for High-Performance Li-Ion and Na-Ion Batteries

A Macromolecule Cathode for High-Performance Li-Ion and Na-Ion Batteries

Bi-Directional H-Bonding Modulated Soft/Hard Polyethylene Glycol-Polyaniline Coated Si-Anode for High-Performance Li-Ion Batteries.

Ultrahigh-capacity silicon (Si) anodes are essential for the escalating energy demands driven by the booming e-transportation and energy storage field. However, their practical applications are strictly hampered by their intrinsically low electroconductivity, sluggish Li-ion diffusion, and undesirably large volume change. Herein, a high-performance Si anode, comprised of a modulated soft/hard coating of polyethylene glycol (PEG) (as Li-ion conductor) and polyaniline (PANI) (as electron conductor) on the surface of Si nanoparticles (NPs) through H-bonding network, is introduced. In this design, the abundant ─OH groups of soft PEG allow it to uniformly cover Si NPs while the hard PANI binds to PEG through its ─N─H group, thus constructing a tight connectin between Si and PEG-PANI (PP). Consequently, the elastic PP allows Si@PP to accommodate the huge volume expansion while possessing fine electronic/ionic conductivity. Therefore, the Si@PP anode exhibits a high initial Coulombic efficiency of 90.5% and a stable capacity of 1871mAhg-1 after 100 cycles at 1Ag-1 with a retention of 85.7%. Additionally, the Si@PP anode also demonstrates a high areal capacity of 3.01mAhcm-2 after 100 cycles at 0.5Ag-1 . This work reveals a scalable interface design of multi-layer multifunctional coatings for high-performance electrode materials in next-generation Li-ion batteries.