Superior Lithium Storage Research Articles

Rational design of ZnS/CoS heterostructures in three dimensional N-doped CNTs for superior lithium storage

Multiphase metal sulfides have proven to show better lithium storage performance than their single phase competitors. However, rational designing of multiphase metal sulfides with rich phase boundaries and heterointerfacial structures is still a big challenge. In this work, a superior structure of nanosized ZnS/CoS heterostructure that embedding in in-situ formed three dimensional N-doped carbon nanotubes frameworks (ZnS/CoS-NCNTs) is fabricated via using a bimetallic zeolitic imidazolate framework (ZnCo-ZIF) as precursor. Due to the crystalline similarity between Zn-ZIF and Co-ZIF, Zn and Co can be uniformly distributed in the ZnCo-ZIF precusor, leading to a uniform distribution of the final nanosized ZnS/CoS heterostructures within NCNTs networks. Therefore, the aggregation of ZnS/CoS heterostructures can be effectively suppressed, resulting in a higher utilization of active materials and improved electrochemical performance. Furthermore, the interconnected NCNTs endow ZnS/CoS-NCNTs with significantly enhanced electronic/ionic conductivity and structural integrity. As a result, the ZnS/CoS-NCNTs exhibits high rate capability and excellent cycling stability, which deliveres high reversible capacities of 1007 mA h g−1 at 1.0 A g−1 after 1000 cycles and 803 mA h g−1 at 5.0 A g−1 after 2000 cycles, respectively.

Nitrogen-rich graphene aerogel with interconnected thousand-layer pancake structure as anode for high performance of lithium-ion batteries

Nitrogen-rich graphene aerogel with interconnected thousand-layer pancake structure (NTLP) was designed and fabricated through hydrothermal template self-assembly method using polystyrene (PS) nanospheres as structural guiding templates and ethylenediamine (EDA) as a nitrogen resource for in-situ N-doping. NTLP exhibits significantly improved electrochemical performance of lithium-ion storage including a highly reversible capacity of 1147 ​mA ​h g−1 at 0.1 ​A ​g−1, and favorable rate capability of 258 ​mA ​h g−1 even at a large current density of 5 ​A ​g−1. Moreover, the reversible capacity is retained at 501 ​mA ​h g−1 after 1100 cycles at 1 ​A ​g−1. PS template effectively alleviates the aggregation of graphene membrane, meanwhile forms peculiar thousand-layered cake structure with high specific surface area and well-controlled pores. Precisely owing to the unique structure with three-dimensionally (3D) interconnected holey graphene network and the introduction of abundant N-doping (about 7 atom%) into the graphene walls, NTLP significantly enhances the electrochemical activity and effectively accelerates the diffusions of both lithium-ions and electrons. The high performance strongly indicates that NTLP possesses a promising perspective for lithium-ion batteries with excellent electronic conductivity, efficient transport pathways of electrons and ions as well as superior reversible lithium storage capacity.

Tetrathiafulvalene-Based Metal-Organic Framework as a High-Performance Anode for Lithium-Ion Batteries.

Metal-organic frameworks (MOFs) have aroused great interest as lithium-ion battery (LIB) electrode materials. In this work, we first report that a pristine three-dimensional tetrathiafulvalene derivatives (TTFs)-based zinc MOF, formulated [Zn2(py-TTF-py)2(BDC)2]·2DMF·H2O (1) (py-TTF-py = 2,6-bis(4'-pyridyl)tetrathiafulvalene and H2BDC = terephthalic acid), can work as a high-performance electrode material for rechargeable LIBs. The TTFs-Zn-MOF 1 electrode displayed a high discharge specific capacity of 1117.4 mA h g-1 at a current density of 200 mA g-1 after 150 cycles along with good reversibility. After undergoing elevated discharging/charging rates, the electrode showed superior lithium storage performance in the extreme case of 20 A g-1 and could finally recover the capability when the current rate was back to 200 mA g-1. Particularly, specific capacities of 884.2, 513.8, and 327.8 mA h g-1 were reached at high current densities of 5, 10, and 20 A g-1 after 180, 175, and 300 cycles along with good reversibility, respectively. Such an excellent performance is first reported for the LIB anode materials. TTFs-Zn-MOF 2, namely, [Zn2(py-TTF-py) (BDC)2]·DMF·2H2O (2), was prepared as a contrast to explore the relationship between the structures of the electrode materials and the electrochemical properties. Based on the structural analysis of 1 and 2 and ex situ X-ray photoelectron spectroscopy, the TTF moiety and the twofold TTF pillar play a key role in the excellent electrochemical performance. The full cell of MOF 1 with NMC 622 delivered the capacity of 131.9 mA h g-1 at 100 mA g-1 with the Coulombic efficiency of 99.45% after 70 cycles and exhibited the tolerance to high-current operation.

Nanostructured LiTi2(PO4)3 anode with superior lithium and sodium storage capability aqueous electrolytes

Aqueous alkali metal ion batteries show great promise as the next generation secondary batteries with low cost, high power density and better safety. However, they suffer from inferior cycle stability at a higher current density and displays poor coulombic efficiency. In this work, LiTi2(PO4)3@C/CNTs (LTP@C/CNTs) with three-dimensional mesoporous nanostructure was investigated in both aqueous lithium-ion batteries (ALIBs) and aqueous sodium-ion battery (ASIBs). Improved rate and cycling performance at high current densities were demonstrated in contrast to LiTi2(PO4)3@C (LTP@C). Typically, the LTP@C/CNTs electrode achieves a discharge capacity of 97.37 mAhg−1 and 90.88 mAhg−1 in ALIBs and ASIBs half cells at 3 A g-1 current density. LTP@C/CNTs//LiMn2O4 and LTP@C/CNTs//Na0.44MnO2 full cells show the capacity retention of 72.9% and 79.4% after 500 cycles. Besides, new electrochemical behavior is reported for the first time, that the anode materials present a two-step sodium ion insertion/extraction in ASIBs. After cycling, LTP anode converts into (NaTi2(PO4)3) NTP phase with maintained crystallinity. LTP@C/CNTs composite anode thus shows a great potential application in next-generation aqueous energy storage systems.

Electrochemically driven amorphization of (Li-)Ti-P-O nanoparticles embedded in porous CNTs for superior lithium storage performance

Amorphous materials have many advantages over their crystalline states in transfering Li+ without restriction of defects, tolerating large volume change during the charging/discharging process and achieving a higher potential in lithium-ion batteries (LIBs). Crystalline LiTi2(PO4)3/TiP2O7 nanoparticles embedded in porous CNTs were constructed firstly by sol-gel and calcination, in which sulfonated polymer nanotubes as both carbon source and template. Afterwards, amorphous (Li-)Ti-P-O nanoparticles embedded in porous CNTs were formed by electrochemical activation. Due to amorphous (Li-)Ti-P-O nanoparticles providing the multi-channel transport of Li+ and the porous carbon matrix preventing the gathering and pulverization of (Li-)Ti-P-O nanoparticles during the electrochemical process, (Li-)Ti-P-O/C hybrid nanotubes exhibit stable cyclic performances and good rate capacities (the capacities of Li-Ti-P-O/C and Ti-P-O/C hybrid nanotubes possess 388.9 and 457.2 mAh g−1 at 0.2 A g−1 after 500 cycles, and maintain 155.0 mAh g−1 at 5 A g−1 after 500 cycles and 123.3 mAh g−1 at 5 A g−1 after 3000 cycles, respectively). This paper provides a feasible method for the preparation of other anode materials with superior lithium storage performance.

Water-soluble salt-templated strategy to regulate mesoporous nanosheets-on-network structure with active mixed-phase CoO/Co3O4 nanosheets on graphene for superior lithium storage

Facile construction of high-energy Li-ion batteries (LIBs) anode materials with robust heterostructure remains great challenges, especially for the fine integration of active materials with conductive carbon. Here, vertically aligned mixed-phase CoO/Co3O4 nanosheets anchored on wrinkled graphene (CoO/Co3O4/Gra) are controllably synthesized with the assistance of water-removable NaCl-templates through facile freeze-drying and calcination processes. In-depth investigations disclose that the wrinkled graphene induces the bonding with nucleating precursors, and the nanosheets vertically grow along the crystal planes of multilevel-NaCl. The as-formed mesoporous nanosheets-on-network structure endows the hybrids with efficient exposure of mixed-phase CoO/Co3O4 active sites and rapid charge-transfer channels. And the multiple composites can integrate the advantages of their long complements and fully exert their synergistic effects to solve the problems of the single metal oxide electrode. Furthermore, the electrochemical performance of hierarchically mesoporous architecture is beyond that of the single individual structure on account of the sufficient electrode/electrolyte interfaces, rapid Li+ diffusion and electron conduction, and stable structural integrity upon cycling. Accordingly, the capacitive kinetic of Li-storage behaviors is greatly enhanced by these synergistic effects. Serving as a LIBs anode material, the mesoporous CoO/Co3O4/Gra-4 hybrid yields superior reversible capacity (1390 mAh g−1 at 0.1 A g−1), high rate performance (1130 mAh g−1 at 0.2 A g−1), and impressive cycling stability (811 mAh g−1 after 500 cycles at 1 A g−1). This work may inspire the design of high-performance electrodes with advanced 3D hierarchical structures.

Highly dispersed SnO2 nanoparticles confined on xylem fiber-derived carbon frameworks as anodes for lithium-ion batteries

Abstract Tin oxide (SnO2) has been considered as a promising alternative material for lithium-ion batteries (LIBs) anodes owing to its high specific capacity, low operation potential and high natural abundance. However, its practical performance is hampered by the poor rate capability and fast capacity fading. In this work, we synthesized the highly dispersed SnO2 nanoparticles confined on the xylem fiber-derived carbon frameworks (SnO2@XFC@C) by a facile solvothermal method. The synergy of using open XFs-derived carbon as conductive framework and glucose-derived carbon as matrix enables the superior lithium storage capability of SnO2 materials. Using aqueous electrode proceeding, the SnO2@XFC@C delivers a high discharge capacity of 1810 mAh g−1 with an initial Coulombic efficiency of 85.4%, and excellent high-rate cycling stability (505 mAh g−1 at 1.0 C after 1000 cycles). This structure design offers significant advantages in terms of realization of low cost, high energy and sustainable lithium-ion batteries, and is extendable to other battery systems.

Metal organic framework derived Co3O4/Co@N–C composite as high-performance anode material for lithium-ion batteries

In this work, a scalable approach of preparing Co3O4/Co@N–C composite derived from metal organic frameworks (MOFs) is developed. After consecutive carbonization and oxidation of MOFs at different calcination temperatures, a series of nanocomposite consisting of Co3O4, conductive Co nanoparticles, and Nitrogen doped (N-doped) mesoporous carbon are obtained via in-situ polymerization strategy. When employed as anode materials for lithium-ion batteries (LIBs), the Crystalline-Co3O4/Co@N–C-700 (Cry-Co3O4/Co@N–C-700) electrode has shown high reversible specific capacity of 896.5 mAh g−1 at 0.1 A g−1, excellent rate capability of 376.2 mAh g−1 at a large current density of 2 A g−1, and robust long-term capacity retention rate of 96.0% at 0.2 A g−1 after 50 cycles. Such superior lithium storage performance could be attributed to the unique porous structure which composed of well-dispersed Co3O4 and conductive Co nanoparticles together with N-doped carbon skeleton. The unique structure can effectively improve the conductivity and act as a buffer medium to alleviate the volume change, which shows potential application for new energy storage materials.

Rosa roxburghii-like hierarchical hollow sandwich-structure C@Fe2O3@C microspheres as second nanomaterialsfor superior lithium storage

Fe2O3, as a promising advanced anode for the next generation lithium ion batteries, behaves high theoretical capacity and rich electrochemical properties. However, the poor cycle performances and low conductivity impede its extensive applications in lithium ion batteries. Herein, the von Mises stress distribution on solid spheres and hollow spheres were simulated by finite element method which confirmed the vital role of porous hollow spheres on strain-relaxation behavior as electrode materials. We also have developed a template method for the first preparation of rosa roxburghii-like hierarchical hollow sandwiched C@Fe2O3@C microspheres as second nanomaterials for superior lithium storage. As an advanced anode for lithium ion batteries, the porous C@Fe2O3@C microspheres exhibit reversible gravimetric capacity (1167 mAh g−1 after 100 cycles at 0.2 C), high rate performance (762 mAh g−1 after 1000 cycles at 1 C) and cycling stability without obvious capacity fading. The excellent performance is ascribed to the hierarchical hollow structure which can better withstand the stress produced in the process of ion embedding/stripping and alleviate the volume change of materials. On the other hand, the double carbon layer can effectively inhibit the self-aggregation effect of nano-scale Fe2O3 and provide a three-dimensional electronic network.

Design of quadruple-layered metal oxides/nitrogen, oxygen-doped carbon nanotube arrays as binder-free electrodes for flexible lithium-ion batteries

Designing flexibly binder-free metal oxide electrodes, which could effectively alleviate the mechanical stress and maintain the structural integrity during the lithiation/delithiation process, is still a major challenge. Here we report a facile strategy for successfully synthesizing free-standing quadruple-layered metal oxides/nitrogen, oxygen-doped carbon nanotube array electrodes. In the quadruple-layered structure, metal oxides are protected by carbon layer to minimize the direct exposure to the electrolyte and accommodate the huge volume change during cycling, and thus form the solid-electrolyte interface layer. Besides that, the abundant oxygen and nitrogen-containing functional groups of carbon layer shows a strong interaction with metal oxides to prevent the electrode pulverization during charging and discharging. Meanwhile, carbon layer is introduced to facilitate the stable and fast electrons mobility. As a result, the as-prepared quadruple-layered electrodes show excellent electrochemical performance in terms of high reversible capacity, good rate capability, and stable cyclability. This work may pave the way for the construction of flexible binder-free lithium ion batteries with superior lithium storage properties.

Unraveling superior lithium storage performance of MnO by a three-dimensional structure-memory anode

MnO is a promising anode material for high-performance lithium-ion batteries (LIBs) due to its high theoretical capacity and rich resource. However, MnO has low electrical conductivity and suffers from drastic volume changes during cycling, resulting in poor cycling stability and limited rate capability. Here, we demonstrate the elaborate design of a novel three-dimensional structure-memory electrode (3D SME) material consisting of MnO nanoparticles encapsulated in the N-doped carbon (NC) as well as anchored on reduced graphene oxide (RGO) nanosheets. The structures of electrolyte diffusion channels, electrode strain-control layer, and electrode/electrolyte interface are all engineered from the ‘memory’ formed during the wet processes. This delicate design rationally combines the compositional and structural merits of NC and MnO species with RGO framework. Consequently, the 3D SME exhibits high specific capacity (927.5 mAh g−1 at 0.1 A g−1), high rare capability (375.3 mAh g−1 at 5.0 A g−1), and long-term cycling stability (835.7 mAh g−1 after 1000 cycles at 2.0 A g−1). Additionally, the charge storage mechanism of 3D SME is investigated by combining ex situ X-ray photoelectron spectroscopy and cyclic voltammetry, revealing a reversible conversion reaction between Mn species and Li+ ions upon the lithiation/delithiation process. This study reports a delicate design to achieve high-performance MnO/C anodes for LIBs, more importantly, provides significant insight into the reaction mechanism of MnO-based anode.

Microsized SnS/Few‐Layer Graphene Composite with Interconnected Nanosized Building Blocks for Superior Volumetric Lithium and Sodium Storage

To develop anode materials with superior volumetric storage is crucial for practical application of lithium/sodium‐ion batteries. Here, we have developed a micro/nanostructured SnS/few‐layer graphene (SnS/FLG) composite by facile scalable plasma milling. Inside the hybrid, SnS nanoparticles are tightly supported by FLG, forming nanosized primary particles as building blocks and assembling to microsized secondary granules. With this unique micro/nanostructure, the SnS/FLG composite possesses a high tap density of 1.98 g cm−3 and thus ensures a high volumetric storage. The combination of SnS nanoparticles and FLG nanosheets can not only enhance the overall electrical conductivity and facilitate the ion diffusion greatly, but alleviate the large volume expansion of SnS effectively and maintain the electrode integrity during cycling. Thus, the densely compacted SnS/FLG composite exhibits superior volumetric lithium and sodium storage, including high volumetric capacities of 1926.5/1051.4 mAh cm−3 at 0.2 A g−1, and high retained capacities of 1754.3/760.3 mAh cm−3 after 500 cycles at 1.0 A g−1. With superior volumetric storage performance and facile scalable synthesis, the SnS/FLG composite can be a promising anode for practical batteries application.

Triple-layered sandwich nanotube of carbon nanotube@TiO2 nanocrystalline@carbon with superior lithium storage performance

The triple-layered sandwich nanotube of carbon nanotube@TiO2 nanocrystalline@carbon is synthesized. TiO2 nanocrystalline stably adheres to carbon nanotubes. A layer of amorphous carbon shell derived by PPy tightly attaches on the surface of TiO2 nanocrystalline. Carbon nanotube@TiO2 nanocrystalline@carbon is of abundant mesopores, showing high pore volume of 0.92 cm3 g−1 and large specific surface area of 612 m2 g−1. As anode material of lithium ion batteries, it exhibits high discharge capacity, desirable cycling performance (236 mA h g−1 at 1C after 500 cycles) and excellent rate capability (187 mA h g−1 at 10C). The outstanding lithium storage performance comes from the supporting effect of the internal carbon nanotube and the protecting effect of the external carbon shell, which significantly increase cycling stability and electronic conductivity of TiO2. The large specific surface area brings about intense pseudocapacitive lithium storage effect, enhancing reversible capacity and rate performance of TiO2.

Large-size carbon-coated SnO2 composite as improved anode material for lithium ion batteries

SnO2 microbelt coating carbon composite was fabricated via electrospinning precursor, thermal treatment, and polymer adhesion process. Primarily, the solvent of electrospinning jet quickly evaporates in a relatively high-temperature environment; intermediate microtubules simultaneously form when the solute containing tin salt and binder converge on the skin of the jet; then, the microtubules collapse into flat microbelt product under the action of atmospheric pressure. Subsequently, SnO2 microbelts can be obtained by annealing the electrospinning products. Finally, the SnO2@C microbelts are synthesized by dopamine polymerization and carbonization process. The SnO2@C microbelts present a regular strip with width ~ 1.2 μm and thickness ~ 120 nm. Because of the synergy effect of carbon coating and SnO2 microbelt design project, the composite shows superior lithium storage of 504 mAh g-1 after 100 cycles at 0.2 A g-1. The SnO2@C microbelts are expected to be competitive alternative anode material of next-generation LIBs.

Spherical-graphite/nano-Mn2O3 composites as advanced anode materials for lithium half/full batteries

The spherical-graphite/Mn2O3 composites (SG/Mn2O3) with a core-shell structure have been facilely synthesized by the initial coprecipitation method and subsequent calcination treatment. As-synthesized composites as anode materials demonstrate remarkable lithium storage performances. The optimal SG/Mn2O3 with 17.6 wt% of Mn2O3 nanoparticles manifests the charge capacity of 499 mA h g−1 over 100 cycles at 0.5 A g−1, and presents the reversible capacity of 383 mA h g−1 under 2 A g−1 after 1000 long cycles for lithium-ion half batteries. When the optimal SG/Mn2O3 electrode is assembled to full-cell using LiFePO4 as the cathode, the full-cell affords the discharge capacity of 318 mA h g−1 with capacity retention of 97.2% at 0.1 A g−1 over 30 cycles. The high capacity of Mn2O3 nanoparticles coating on the surface/interface of SG enhances the long-periodic cycling properties and rate performance of overall electrode. The superior lithium storage performance demonstrates that the SG/Mn2O3 has great potential in the new-generation energy storage devices.

Facile One-Step Preparation of 3D Nanoporous Cu/Cu6Sn5 Microparticles as Anode Material for Lithium-Ion Batteries with Superior Lithium Storage Properties

In this article, three-dimensional nanoporous Cu/Cu6Sn5 microparticles (3D-NP Cu/Cu6Sn5 MPs) were prepared by one-step chemical dealloying of Cu20Sn80 (at%) alloy slices in a mixed aqueous solution of HF and HNO3 and then filled into a three-dimensional porous copper foam (3D-PCF) skeleton as anode (3D-PCF@Cu/Cu6Sn5) for lithium-ion batteries (LIBs). The results show that the ellipsoidal 3D-NP Cu/Cu6Sn5 MPs with feature sizes of 3 to 8 μm are composed of numerous uniform nanoparticles (100 to 200 nm) and plenty of voids. Compared with similar Sn-based electrodes in this work and other published reports, the as-prepared electrode delivers more outstanding electrochemical performance with a superior reversible capacity of 1.90 mAh cm−2, 84.44% capacity retention and > 99.5% coulombic efficiency upon 200 cycles. The cycling stability and integrity of the overall structure of the composite electrode have been greatly enhanced under the synergistic effect of the buffer effect of copper as the inactive component, the unique hierarchical porous electrode architecture and the effective limitation in three dimensions of the 3D-PCF skeleton. We are confident that this work can provide new-generation LIBs with a promising anode candidate and a facile method of dealloying, and a subsequent filling step can achieve the practical production and application of high-performance LIBs.

Zinc Oxide Quantum Dots Embedded Porous Carbon Nanosheets for High-Capacity and Ultrastable Lithium-Ion Battery Anodes

Summary Carbon materials are widely used in lithium-ion batteries (LIBs) due to their high performance, safety, and reliability, along with low cost and easy availability. However, the low lithium storage capability of bare carbon materials limits the further improvement of the capacity of LIBs. Here, we report a facile self-poring strategy for the synthesis of trace amounts of ZnO quantum dots (QDs) (∼5 nm) embedded in highly porous carbon nanosheets by using the metal centers of a Zn-based metal-organic ligand structure as a pore-creating agent. Benefiting from the synergistic functions of nanostructuring, heterocomponent doping, and QDs effects, the as-prepared materials deliver superior lithium storage properties in comparison with the existing carbon-based materials—2,300 mAh g−1 at 0.2 A g−1, ∼600 mAh g−1 at 10 A g−1, and ∼700 mAh g−1 after 3,000 cycles at 5 A g−1—and are promising candidates for next-generation high-capacity LIB electrodes.

Dual-metal-organic frameworks derived manganese and zinc oxides nanohybrids as high performance anodes for lithium-ion batteries

Metal-organic framework (MOF) derivatives are attracting increasing interests for next-generation lithium-ion battery anode materials. Here, a novel approach has been applied to synthesize binary Mn–Zn oxides nanohybrids embedded in porous carbon matrix by pyrolysis of dual-metal-organic frameworks. The as-fabricated MnO/ZnO@C nanohybrids exhibit superior lithium storage capabilities, reaching a reversible capacity of 1396 mAh g−1 at 0.2 A g−1 with an initial coulombic efficiency of higher than 75%. When cycled at 2 A g−1, the electrode maintained at 636 mAh g−1 after 1000 cycles, indicating the outstanding high-rate capability and cycling stability. The improved electrochemical performance can be attributed to the interconnected porous structure of carbon frameworks and uniform heterostructure nanohybrids, which efficiently improve the charge transfer and buffer the volume expansion during repeated lithiation process. These findings demonstrate an efficient strategy of using dual-MOF-derived bi-metal oxide nanostructures as high performance anodes for lithium-ion batteries.

Construction of CoP@C embedded into N/S-co-doped porous carbon sheets for superior lithium and sodium storage

To improve the electrical conductivity and relief the large volume variation, carbon coated CoP particles were designed to homogeneously embed into porous carbon sheets, which were synthesized though a simultaneous carbonization and phosphorization method. Notably, the uniform carbon shells and porous carbon sheets constructed a tough conductive matrix to enhance the electron transfer and structural stability during charging/discharging processes. Moreover, the heteroatom doping of nitrogen and sulfur could not only introduce more active sites and defects on the carbon sheets, but also increased electrical conductivity. Owing to the unique structure, the obtained material displayed good electrochemical performance for lithium storage (638.8 mA h g−1 at 0.2 A g−1 after 500 cycles and 334.9 mA h g−1 at 10 A g−1) and sodium storage (329.4 mA h g−1 at 0.2 A g−1 after 150 cycles and 162.4 mA h g−1 at 5 A g−1). More importantly, the reaction mechanism and the ion diffusion coefficient were explored by ex-situ XRD and EIS for both LIBs and SIBs. This versatile approach may avail to predigest the tedious phosphating process to obtain high-performance TMPs-based hybrids (such as Ni2P/C) by employing other metal salts.

Crystalline and amorphous carbon double-modified silicon anode: Towards large-scale production and superior lithium storage performance

Carbon coating could suppress the volume expansion of silicon toward high-capacity anode materials for lithium-ion batteries. However, whether crystal carbon or amorphous carbon coating always bring new problems to hinder the industrial application. Crystal carbon could not effectively inhibit the volume expansion, and amorphous carbon-coated silicon has low coulombic efficiency. To solve these defects, we prepared the hierarchical structure material (2-BM) of crystalline carbon and amorphous carbon cascade-coated nano-silicon by a simple and easily mass-produced ball milling method. The 2-BM electrode exhibits ~89% initial coulombic efficiency (ICE) and high reversible capacity of 874.5 mAh g−1 after 300 cycles. Various characterizations demonstrated that the superior electrochemical performances of 2-BM mainly benefit from the hierarchical structure, which not only effectively relieves the volume expansion of silicon, but also facilitates the formation of a thin and stable solid electrolyte interface (SEI) film. The easy-to-manufacture hierarchical structure accelerates the industrialization of silicon-carbon materials.