Anode For LIBs Research Articles

Three-dimensional graphitic hierarchical porous carbon-supported SnOx@nitrogen-doped carbon composite as high-performance lithium ion battery anode material

Utilizing tin and its oxides (SnOx, x = 0/1/2) as anode confront the main problems like large volume expansion and poor electrical conductivity during cycling. As an efficient solution, a three-dimensional (3D) graphitic hierarchical porous carbon (HPC) with highly fluffy structure was employed as a support for fabrication of HPC/SnOx@nitrogen-doped carbon (NC) composite. The resulting HPC/SnOx@NC composite presented an effective dual‑carbon confinement structure with 3D conductive network and high-quality carbon coatings. The unique structure played significant roles in restricting the expansion of Sn and its oxides as well as enhancing their ion/electron transport efficiency. The as-prepared composite exhibited a maintained reversible specific capacity of 644 mAh g−1 after 200 cycles at 1000 mA g−1. In addition, it presented a high specific capacity of 1458 mAh g−1 at 100 mA g−1 and 858 mAh g−1 at 5000 mA g−1 (58.8 % capacitance retention), and meanwhile showed a remarkable cycling stability with a high capacity retention of 63 % (333 mAh g−1) after 850 cycles at 5000 mA g−1. Therefore, the HPC/SnOx@NC composite has the potential to be a new generation of LIBs anode.

Application of carbon and silicon nanomaterials in lithium ion battery anode

The world is in an era of increasing energy demand to meet the development needs of modern society. Both nanotechnology and lithium-ion battery technology play an important role in helping the world meet the growing challenges of energy and environmental problems. In this paper, through consulting relevant materials and referring to relevant papers, the influence and progress of nanostructured electrode materials on the design, synthesis and electrochemical performance of Li-ion battery anode materials are comprehensively introduced. Nanomaterials exhibit unique properties that present intriguing prospects for their use in various sectors. Traditional anodes in LIBs suffer from limited charge capacity, poor cycle life. By reducing the size to nanoscale, these structures can better accommodate the volume changes, hence improving durability and charge capacity. Despite current challenges in terms of cost and scalability, the progress in this field suggests the potential for future advancements in high-performance LIBs with the integration of nanostructured anodes.

Waste to Wealth Approach: Customizing Spent LiB Anodes to High Performance Supercapacitor Electrode

AbstractLithium‐ion batteries (LiBs) are widely used in various applications because of their high energy density, low self‐discharge rate, and portability. The requirements for LiBs continue to increase drastically every year; however, the disposal of spent LIBs is a cumbersome task. To resolve this issue, spent LiB anodes are customized into high‐performance supercapacitor (SC) electrodes via supercritical water exfoliation. The specific capacitance of spent LiB anodes (289 F g−1 at 2 A g−1) significantly improved after exfoliation (351 F g−1 at 2 A g−1). Furthermore, the electrochemical performance of the exfoliated LiB anode mushroomed upon the addition of dopamine (as a redox‐additive for the first time) with a conventional H2SO4 electrolyte. The specific capacitance of the exfoliated LiB anode is incredibly improved after the addition of dopamine with H2SO4, from 286 to 571 F g−1 at 4 A g−1. A flexible SC is also fabricated using PVA/H2SO4 and dopamine/PVA/H2SO4 as the gel electrolyte. The fabricated flexible SC with dopamine/PVA/H2SO4 exhibited an enormously high energy density of 44 Wh kg−1 at 700 W kg−1. The increased specific capacitance and energy density of the SC after the addition of dopamine with H2SO4 and PVA/H2SO4 may be due to the reversible reaction of dopamine to dopamine‐o‐quinone with H+ ions.

MgV3O8 incorporated carbon nanofibers as anode material for high-performance lithium-ion batteries

The rich redox chemistry of vanadate-based materials makes them a potential anode for the fabrication of advanced lithium-ion batteries (LiBs). However, poor electrical conductivity as well as volume variation of vanadate-based anode materials hinders practical applications. Herein, magnesium vanadate (MgV3O8) incorporated carbon nanofibers (CNFs) (MgVO@CNFs) composites were prepared via a simple and scalable electrospinning technique, followed by pyrolysis. The synergistic effect of MgVO and CNFs effectively offers a good conductive path and excellent integrity between the active particles with highly porous network. As an anode for LiBs, the MgVO@CNFs composite electrode exhibited good discharge capacity values of 457 mA h g−1 (over 300 cycles) and 245 mA h g−1 (over 500 cycles) at 0.1 and 0.5 A g−1, respectively and revealed excellent rate performance. The charge storage mechanism of MgVO@CNFs is contributed by both capacitive and diffusion-controlled behaviors. Consequently, this novel preparation process of the MgVO@CNFs may provide a new idea for the fabrication of different kinds of nanostructures for LiB applications.

Bimetallic alloy FexCo1-xPS3 with boosted lithium reaction kinetics for lithium-ion batteries

Metal phosphorous trisulfide (MPS3) is considered to be the promising anode material for LIBs owing to the advantage of its high capacity and layered structure. Nevertheless, the inferior reaction kinetics resulting from its low electron conductivity hinder its further practical application. Herein, bimetallic alloy FexCo1-xPS3 with gradient Fe: Co coated by a nitrogen-doped carbon layer is designed to accelerate the electron transfer and Li-ion diffusion rate. The in-situ X-ray diffraction technique is applied to precisely confirm the phase evolution of the Fe0.63Co0.37PS3 coated by N-doped carbon layer (FCPS-5/NC) anode upon the (de)lithiation process. Theoretical calculations confirm that alloying with Co can reduce the bandgap and decrease the energy barrier of Li ion diffusion. In addition, the conductive carbon layer can improve the electric conductivity of the whole electrode. As an anode for LIBs, the FCPS-5/NC electrode reveals a high rate capacity of 554 mA h g−1 at 3.0 A/g and thus achieves a comparable lithium storage performance among the reported MPS3-based anodes. Meanwhile, the Li-ion full cell assembled with FCPS-5/NC anode also exhibited excellent cycling performance, confirming its value for practical application. This work demonstrates a brand-new strategy to prepare advanced MPS3-based materials for superior LIBs.

Nano GeSe2/C anchored in carbon sponge skeleton for free-standing flexible lithium-ion battery electrodes

As a typical conversion alloyed anode material, Germanium selenide (GeSe2) exhibits isotropic lithiation behavior and high theoretical charge-discharge specific capacity. However, pure GeSe2 anode faces significant volume expansion (∼250 %−360 %) and further exploration is needed in the preparation of flexible electrode materials and structural design. Herein, a simple strategy is designed to load GeSe2/C-2 nanoparticles with porous carbon-coated structure on a flexible cross-networking substrate. The 3D network substrate is composed of highly conductive carbon nanotubes and adhesive cotton cellulose fibers. A two-step method involving coating and cross-linking is designed to achieve the fabrication of self-supporting flexible electrodes. As an anode for LIBs, the one layer GeSe2 discs with ∼0.65 mm thickness manifest capacities of 827.1, 744.4, 676.3, and 472.9 mAh g−1 at 0.1, 0.2, 0.5, and 1 A g−1, respectively. This superior Li+ storage performance can be attributed to the positive collective impact from the integration of nano-scale material, low crystalline properties, and carbon sponge skeleton. Furthermore, the GITT tests indicate that the diffusion coefficient of Li+ in the GeSe2-based electrodes ranged from 10−15 to 10−12 cm2/s, and the thickness of the flexible electrode (including two layers) has a negligible impact on its electrochemical performance.

Explore the feasibility of Janus 2H-VSeTe monolayer as anode material for Li ion battery

Two-dimensional (2D) materials as potential energy storage systems have received extensive attention due to their high energy density and rate performance. Here, the electronic properties and feasibility of Janus 2H-VSeTe monolayer as LIBs anode material are systematically investigated using the first-principles calculations. No imaginary frequency in the phonon spectrum and the absence of obvious deformation simulated by AIMD simulations at 300 K prove the dynamic and thermal stability of Janus 2H-VSeTe monolayer, respectively. The pure Janus 2H-VSeTe monolayer exhibits a small direct band gap semiconductor character. The Li atom adsorption can result in the increase of electronic states near Ef and a transform of metallic behavior, ensuring good conductivity for the Janus 2H-VSeTe monolayer. On the other hand, the adsorbed Li atoms are fully ionized to ensure the charge and discharge process by the Bader analysis. Through the climbing-image nudged elastic band method, two possible migration paths are considered on the Se and Te surfaces, respectively. The lowest potential barriers are 0.159 eV and 0.188 eV, respectively, which proves that there is a high ion migration rate during charge and discharge process. The OCV and multi-layer Li atoms adsorption suggest that the corresponding specific capacity is 416 mA h g−1 for the Janus 2H-VSeTe monolayer, which reveals that Janus 2H-VSeTe monolayer is one of the feasible candidates for LIBs anode materials.

Constructing superior rate-performance manganese-based anode for lithium-ion batteries by tuning interface effect

Interface engineering is an effective way to improve the electrochemical performance of electrode materials for LIBs. Point contact interfaces in composites are constructed by growing of Mn3O4 nanoparticles on the surface of acetylene black (AB). The prepared electrode materials exhibit excellent rate capability (355.7 mAh g−1 at 6.4 A g−1) and cycling stability (1386.7 mAh g−1 after 300 cycles at 1 A g−1). The presence of AB in the composite reduces the charge transfer resistance and improves the cycling stability of the electrode. Moreover, the interface between the composites increases the contribution of pseudocapacitance, which will facilitate the electrode kinetics. The construction of interfaces in the composites provides a promising perspective for the design of high-power density anode for LIBs. Highlights Construction of Mn3O4 nanoparticles on 0 D-AB spheres was proposed and synthesised by a facile and scalable strategy. The composite materials exhibit excellent electrochemical performance. The superior rate performance is mainly attributed to the interface effect of composite material.

Facile synthesis of Fe3O4 ultrathin layer coated Fe2O3 composite anode for enhanced lithium-ion storage

Fe2O3 has been considered as a promising anode material for lithium-ion batteries (LIBs) owing to its high specific capacity. However, its sluggish charge transfer resulting from the poor electrical conductivity severely limits the electrochemical performance. In this work, an ultrathin Fe3O4 layer-coated Fe2O3 composite was fabricated through a facile one-step hydrothermal method with hydrazine hydrate as the reductant in an alkaline environment. Upon use as the anode for LIBS, the as-resulted Fe2O3@Fe3O4 composite achieves a high specific capacity of 1539.5 mA h g−1 at a current density of 100 mA g−1 and simultaneously maintains a high discharge capacity of 707.8 mAh g−1 after 800 cycles at 1000 mA g−1, outperforming the commercial Fe2O3 sample. Electrochemical characterizations reveal that the improved electrochemical performance can be attributed to the combined effects of higher theoretical specific capacity of Fe2O3 and superior electrical conductivity of Fe3O4.

Carbon-coated SiO for LIBs with superior capacity and cycle stability

Silicon monoxide (SiO) is suggested as anode for LIBs with excellent theoretical capacity. Unfortunately, the low electrical conductivity and volume expansion limit its practical application. The preparation of SiO@C composites can effectively solve these problems. SiO@C composite materials are constructed with phenolic resin pyrolysis method. Experimental data indicate that SiO@C-20 with carbon content of 20 wt% possesses a high discharge capacity and superior initial coulombic efficiency (74.81 %) compared to others. The superior performance can be attributed mainly to carbon ratio with adjusting phenolic resin.

Simple ball milling-assisted method enabling N-doped carbon embedded Si for high performance lithium-ion battery anode

Si has been regarded as a hopeful advanced anode of lithium-ion batteries due to its features such as ultrahigh theoretical specific capacity and high natural abundance. But, it suffers from electrochemical irreversibility because of large volumetric change and poor conductivity during cycle. In spite of obtaining enhanced lithium storage performance after compositing with carbon materials, most of the reported Si/C composite anodes lack a simple preparation process. For the new anode materials, the simple preparation process is as important as showing high performance. Herein, an efficient simple method is developed to prepare a composite of N-doped carbon embedding Si nanoparticles (Si@C) to response to the above Si faced challenges. Its preparation process just consists of very simple ball milling and pyrolysis carbonization, showing great simplicity. The findings confirm that the combination of the ball-milling mixing and the use of PVP carbon precursor enables the optimal Si@C-2 composite to have a N-doped carbon embedding structure and a robust interface Si-O-C chemical bond bonding, hence obtaining enhanced conductivity, high electrochemical kinetics and superb structure stability during cycling process. Therefore, the Si@C-2 anode exhibits excellent performance, with 1542 and 794.7 mA h g−1 after 100 and 1000 cycles at 100 and 1000 mA g−1, respectively, superior to many reported Si/C composites. The simple, scalable preparation method and superb performances offer Si@C-2 great promising in advanced LIB anode applications.

Solution-catalyzed carbothermal reduction of argo-waste SiO2 enables low-temperature and fast synthesis of Si(Ⅱ)-C anode

Divalent silicon composite materials are becoming increasingly important in the anode industry of lithium-ion battery. However, the preparation of silicon(Ⅱ) composite materials based on traditional carbothermal reduction and comproportionation faces high operation temperature, high energy consumption, and relatively slow reaction rate due to strong Si-O covalent bonds and solid-state reaction process. Here, we report an efficient carbothermal reduction strategy to achieve low-temperature synthesis of carbon-based silicon(Ⅱ) composite from argo-waste SiO2 by introducing molten alloys as solution-catalytic reaction media. During the reaction process, the selected Sn-based molten alloys simultaneously extract SiO2 and highly active carbon from straws, thus facilitating the dissociation of Si-O bonds and further catalyzing the carbothermal reduction. Importantly, compared with traditional solid phase reaction, the Sn-based solution-catalytic environment can greatly accelerate the reaction rate. Without using highly reactive metal such as Al and Mg, low oxygen-potential Sn-based molten alloy catalyst can be easily separated from the product, recycled and regenerated, thus significantly simplifying the preparation process. Benefitting from the structure merits of biomass, the resulting carbon silicon(Ⅱ) composite as a LIB anode exhibits high reversible capacity, good rate capability and excellent cycling stability.

Exfoliability of two-dimensional silicon nanosheets from calcium disilicide and its enhanced performance as lithium-ion battery anode material

Two-dimensional silicon nanosheets are a promising pathway for achieving stable silicon anode materials due to their large specific surface area, lower diffusion energy barrier, and controlled volume change. The soft chemical topochemical reaction of calcium disilicide is a top-down approach for synthesizing silicon nanosheets of interest due to its potential for large-scale applications. However, the as-reacted material is composed of multilayer silicon nanosheets still held together by interlayer Van der Waal forces which limit its performance and cycling stability as LIB anode material. The current work investigates the exfoliation of soft topochemical-synthesized 2D silicon nanosheets, and a strategy for controlling nanosheet morphology, exfoliability, yields, and LIB performance is outlined herein. The soft topochemical reaction for the top-down synthesis of silicon nanosheets in anhydrous ethanol demonstrates improved exfoliability and initial specific capacities of up to 2390 mAh/g and retentions up to 96.6 % (200 cycles). The exfoliation mechanism and yields were discussed concerning the underlying solute-solvent interactions and sonication hydrodynamic cavitation. Exfoliation yields of up to 10 % are achieved, which is higher than any other reported in the literature for soft chemical synthesis, thus demonstrating the process' potential for large-scale applications.

A 3D Multilevel Heterostructure Containing 2D Vertically Aligned MoS2 Nanosheets and 1D Sandwich C-MoS2-C Nanotubes to Enhance the Storage of Li+ Ions.

To overcome the disadvantages of the MoS2 anode for LIBs in terms of low intrinsic conductivity, poor mechanical stability, and adverse reaction with electrolytes, a 3D multilevel heterostructure (VANS-MoS2-CNTs) has been successfully prepared by a simple hydrothermal method followed by thermal treatment. VANS-MoS2-CNTs are made up of 2D vertically aligned MoS2 nanosheets (VANS) and 1D sandwich C-MoS2-C nanotubes (CNTs). The sandwich-like nanotube is the core part, which is made up of the MoS2 nanotube covered by carbon layers on both side surfaces. Due to the special heterostructure, VANS-MoS2-CNTs have good conductivity, high structured stability, and excellent Li+/electron transport, resulting in high discharge capacity (1587 mAh/g at a current density of 0.1 A/g), excellent rate capacity (1330 and 730 mAh/g at current densities of 0.1 and 2 A/g, respectively), and good cyclic stability (1270 mAh/g at 0.1 A/g after 100 cycles).

Ice template induced assembly strategy for preparation of 3D porous carbon frameworks from low-cost carbon quantum dots for high-performance lithium-ion batteries

Consider the natural similarities between the structures of coal tar pitch and carbon quantum dots (CQDs), the mass-production of low-cost zero-dimensional (0D) CQDs was achieved by using the mild oxidation with hydrogen peroxide (H2O2). The as-obtained CQDs possesses a uniformly distributed size with a diameter of 4.16 ± 0.46 nm, many oxygen-containing functional groups, distinct crystallinity nature and a production yield of ∼18 wt%. Subsequently, ice-template induced assembly coupled with carbonization strategy reveals a transition from 0D CQDs to 3D porous carbon frameworks. Differing from the well-defined porous carbon, the obtained porous carbon frameworks consist of cross-linked and twisted nanosheets, achieving a well-developed hierarchical porous structure with a reasonable specific surface area and a gradient distribution of meso/micropores. LIBs based on porous carbon frameworks as anode materials show excellent long-cycle performance, as evidenced by reversible capacity of up to 273 mAh·g−1 after 1000 charge-discharge cycles at 2000 mA·g−1. The research emphasizes a green method of preparing CQDs from representative low-value coal tar pitch and the directional transition from 0D CQDs to 3D porous carbon frameworks, providing a promising idea to prepare functional carbon materials and endow them opportunities for LIBs anode.

Bi nanoparticles with different oxidation states embedded in porous carbon nanosheets as high-performance anode for lithium-ion battery

Bi-based material is a new candidate anode for LIBs. Herein, we fabricate Bi nanoparticles (NPs) with different oxidation states embedded in mesoporous carbon matrix based on bismuth citrate-engaged etching-pyrolysis strategies. For Bi@MCNSs-500, the oxidation state of Bi is Bi3+. Nevertheless, for Bi@MCNSs-700 and Bi@MCNSs-900, Bi appears as a metallic phase (Bi0 and Bi3+). Bi@MCNSs-700 shows excellent electrochemical properties as anode material for LIBs. Bi@MCNSs-700 has an initial discharge capacity of 1422.65 mAh g−1 at 0.05 A g−1 and it exhibits high capacity of 312 mAh g−1 at 5 A g−1, and exhibits excellent cycling performance (1 A g−1, 393.2 mAh g−1 after 1000 cycles). Such extraordinary performances are attributed to (1) ultra-small Bi NPs and suitable oxidation states can provide massive active sites and facilitate Li+ storage. (2) the porous carbon nanosheets can improve the conductivity, and effectively offer sufficient space to adapt to volume changes during cycling, thus improving cycling stability for Li+ storage. This work provides perspective into the design of excellent Bi-based materials for LIBs.

Facile Synthesis of Nickel Phosphide @ N-Doped Carbon Nanorods with Exceptional Cycling Stability as Li-Ion and Na-Ion Battery Anode Material

Nickel phosphide (Ni2P), as an anode material for both lithium- and sodium-ion batteries, offers high theoretical specific and volumetric capacities. However, considerable challenges include its limited rate capability and low cycle stability arising from its volume change and degradation during cycling. To solve these issues, appropriate composite micro/nanoparticle designs can improve conductivity and provide confinement. Herein, we report a simple pyrolysis method to synthesize nitrogen-doped carbon-coated Ni2P nanorod arrays (Ni2P@NC) from nickel foam and an ionic resin as a source of carbon, nitrogen and phosphorus. The N-doped open-ended carbon shells provide Ni2P containment, good electrical conductivity, efficient electrolyte access and the buffering of bulk strain during cycling. Consequently, as a LIB anode material, Ni2P@NC has impressive specific capacity in long-term cycling (630 mAh g−1 for 150 cycles at 0.1 A g−1) and a high rate capability of 170 mAh g−1 for 6000 cycles at 5 A g−1. Similarly, as a SIB anode, Ni2P@NC retains a sizable 288 mAh g−1 over 300 cycles at 0.1 A g−1, and 150 mAh g−1 over 2000 cycles at 2 A g−1. Furthermore, due to a sizable portion of its capacity coinciding with adequately low voltage, the material shows promise for high volumetric energy storage in full-cell format. Lastly, the simple synthesis method has the potential to produce other carbon-coated metal phosphides for electrochemical applications.

Innovative BVO@CuO design: A high-performance vanadium-based anode material for Li-ion batteries

Herein, a specific structure of BVO coated on CuO@Cu current collector (denoted as BVO@CuO) was constructed in the study by merging a metal oxide (hollow cubic structure BiVO4) and a lithiophilic oxide (lithiophilic copper oxide array). The design-specific structure was recovered and a high-performance composite anode for LIBs (referred to as r-BVO@CuO) was built using a straightforward preferential reduction technique. Specifically, the lithiophilic copper oxide array is reduced to the nano-copper array, and the reduction products Bi and Li3VO4 of BVO are embedded in the nano-copper array. This structure can not only buffer the volume expansion of Bi during the transformation of Li and Bi into alloy but also prevents the dissolution of Li3VO4, which helps improve the cycle stability of the electrode and maintains a high capacity. At the same time, some copper particles enter into the electrode material, which has enhanced the electronic conductivity of the anode and improved the rate performance of the LIBs. Therefore, the r-BVO@CuO shows an excellent reversible capacity of 1052 mAh g−1 at 0.1 A g−1 (The theoretical capacity of graphite is 372 mAh g−1). The capacity retention of r-BVO@CuO is about 90.5% after 100 charge/discharge cycles. Meanwhile, X-ray diffraction and density functional calculation analyses are employed to demonstrate the alloy change process of r-BVO@CuO during electrochemical cycling. Subsequently, LIB full cells are constructed with r-BVO@CuO as the anode and lithium iron phosphate as the cathode assembly (denoted as LFP|r-BVO@CuO LIBs). The devices can reach ∼ 165 mAh g−1 at 1 C, which is higher than LFP|Li LIBs (140 mAh g−1) and LFP|r-BVO LIBs (90 mAh g−1). Although the voltage plateau of LFP|r-BVO@CuO LIBs is comparatively lower than that of LFP|Li LIBs, the energy density (413.8 Wh kg−1) is not significantly different from that of LFP|Li LIBs (449.9 Wh kg−1), for the cathode only. Interestingly, the device delivers a capacity of 134 mAh g−1 after 1100 charge-discharge cycles with a capacity retention of 85.3%. This work may be widely applied to manufacture BVO-type anodes to improve electrochemical performance in energy-related storage-related fields.

Van der Waals Forces between S and P Ions at the CoP‐C@MoS2/C Heterointerface with Enhanced Lithium/Sodium Storage

AbstractMetal–organic framework‐derived metal phosphides with high capacity, facile synthesis, and morphology‐controlled are considered as potential anodes for lithium/sodium‐ion batteries. However, the severe volume expansion during cycling can cause the electrode material to collapse and reduce the cycle life. Here, novel CoP‐C@MoS2/C nanocube composites are synthesized by vapor‐phase phosphating and hydrothermal process. As the anode of LIBs, CoP‐C@MoS2/C exhibits outstanding long‐cycle performance of 369 mAh g−1 at 10 A g−1 after 2000 cycles. In SIBs, the composite also displays excellent rate capability of 234 mAh g−1 at 5 A g−1 and an ultra‐high the capacity retention rate of 90.16% at 1 A g−1 after 1000 cycles. Through density functional theory, it is found that the S ions and P ions at the interface formed by CoP and MoS2 can serve as Na+/Li+ diffusion channels with an action of van der Waals force, have attractive characteristics such as high ion adsorption energy, low expansion rate and fast diffusion kinetics compared with MoS2. This study provides enlightenment for the reasonable design and development of lithium/sodium storage anode materials composited with MOF‐derived metal phosphides and metal sulfides.

Interplanar Spacing Engineering on Copper‐Benzenedicarboxylate Toward Stabilized Lithium Storage

Metal–organic frameworks (MOFs) have drawn intensive attention for their prospect as electrode materials of lithium‐ion batteries. However, MOFs with high capacity usually suffer from poor cycling stability, due to the volume fluctuation during cycles. Herein, based on the structure tenability of MOFs, copper phthalate (Cu‐oBDC), copper isophthalate (Cu‐mBDC), and copper terephthalate (Cu‐pBDC) with the same active sites for lithium storage are chosen as target materials and investigated as anodes for LIBs. The three MOF materials display different cycle stability in the galvanostatic charge–discharge test. Cu‐mBDC and Cu‐pBDC show obvious performance attenuation in cycles, while Cu‐oBDC with the largest interplanar spacing (13.02 Å) is eventually stabilized, and the solid electrolyte interface membrane is formed in the later cycling. At a current density of 100 mA g−1, the Cu‐oBDC delivers a reversible specific discharge capacity of 683.6 mAh g−1after 250 cycles, outperforming the other two counterparts. This work adjusts the crystal structure of MOFs toward the improvement of cycle stability and provides a strategy to optimize the electrochemical performances of MOFs.