High Reversible Capacity Research Articles

Electrospun MOF-derived N-doped mesoporous carbon fibers embedded with ultrafine vanadium oxide as an ultralong cycling stability for potassium ion storage

Potassium-ion batteries (KIBs) are promising options for large-scale energy storage because of their low cost and low redox potential. The use of anodes with porous structures is an attractive strategy to improve the electrochemical properties of KIBs. However, the development of KIB anodes has been hindered by their low capacity and difficulty in synthesizing porous structures. Herein, ultrafine vanadium oxide nanoparticles embedded in porous N-doped carbon nanofibers (VO@PNCNFs) using electrospinning and one-step heat treatment are reported. The uniform growth of vanadium oxide crystals is facilitated by the porous structure of the carbon nanofiber. The numerous pores play a crucial role in the transfer of electrons and ions and provide structural stability to the N-doped carbon matrix. As a result, the VO@PNCNF electrode demonstrates a high reversible capacity (∼205 mA h g−1 at 1.0 A g−1), good cycle stability over 3000 cycles, and excellent rate performance (95 mA h g−1 at 3.0 A g−1).

Nickel-doped CNTs composite as cathode by sulfur vapor deposition for high-performance all-solid-state lithium‑sulfur batteries

Shuttle effect of polysulfide in the cathode and the safety issues arising from dendrite formation at Li metal anode are the main challenges of traditional liquid lithium‑sulfur batteries. In order to solve the shuttle effect and prevent short circuit, the all-solid-state lithium‑sulfur battery (ASSLSB) is proposed. However, the huge volume expansion of sulfur and the improvement of sulfur conversion efficiency during charge and discharge, which could lead to the limitation of electrochemical performance. Herein, a homogeneous Ni-doped carbon-nanotubes (H-Ni-SVD@CNT) composite cathode of ASSLSB is prepared by sulfur vapor deposition to confine sulfur and promote the conversion of sulfur and Li2S. In this work, SVD-5-S@CNT composite cathode demonstrates high reversible discharge capacity of 1001.1 mAh g−1 after 127 cycles and capacity retention rate of 78.6 % at the rate of 0.1C and 60 °C. Moreover, H-Ni-SVD@CNT composite cathode exhibits superior electrochemical performance, displaying the discharge specific capacity of 1519.3 mAh g−1 at 0.1C and 60 °C. Meanwhile, the discharge specific capacity of H-Ni-SVD@CNT composite cathode is 1060.9 mAh g−1 at room temperature. The synergistic effect of physical confinement and chemical catalysis improves the electrochemical performance of the all-solid-state lithium‑sulfur battery. This work proposes a new strategy for the cathode structure design of the all-solid-state lithium‑sulfur battery.

Manipulating Atomic‐Coupling in Dual‐Cavity Boride Nanoreactor to Achieve Hierarchical Catalytic Engineering for Sulfur Cathode

AbstractThe catalytic process of Li2S formation is considered a key pathway to enhance the kinetics of lithium‐sulfur batteries. Due to the system‘s complexity, the catalytic behavior is uncertain, posing significant challenges for predicting activity. Herein, we report a novel cascaded dual‐cavity nanoreactor (NiCo−B) by controlling reaction kinetics, providing an opportunity for achieving hierarchical catalytic behavior. Through experimental and theoretical analysis, the multilevel structure can effectively suppress polysulfides dissolution and accelerate sulfur conversion. Furthermore, we differentiate the adsorption (B−S) and catalytic effect (Co−S) in NiCo−B, avoiding catalyst deactivation caused by excessive adsorption. As a result, the as‐prepared battery displays high reversible capacity, even with sulfur loading of 13.2 mg cm−2 (E/S=4 μl mg−1), the areal capacity can reach 18.7 mAh cm−2.

Manipulating Atomic-Coupling in Dual-Cavity Boride Nanoreactor to Achieve Hierarchical Catalytic Engineering for Sulfur Cathode.

The catalytic process of Li2S formation is considered a key pathway to enhance the kinetics of lithium-sulfur batteries. Due to the system's complexity, the catalytic behavior is uncertain, posing significant challenges for predicting activity. Herein, we report a novel cascaded dual-cavity nanoreactor (NiCo-B) by controlling reaction kinetics, providing an opportunity for achieving hierarchical catalytic behavior. Through experimental and theoretical analysis, the multilevel structure can effectively suppress polysulfides dissolution and accelerate sulfur conversion. Furthermore, we differentiate the adsorption (B-S) and catalytic effect (Co-S) in NiCo-B, avoiding catalyst deactivation caused by excessive adsorption. As a result, the as-prepared battery displays high reversible capacity, even with sulfur loading of 13.2 mg cm-2 (E/S=4 μl mg-1), the areal capacity can reach 18.7 mAh cm-2.

Tuning the microstructure of biomass-derived hard carbons by controlling the impurity removal process for enhanced Na ion storage performance

Biomass-derived hard carbons are promising anode materials of sodium-ion batteries (SIBs) due to their low cost, renewability and high specific capacity. However, there are inevitably some impurities in biomasses that may not only affect the purity, but microstructure and electrochemical performance of hard carbons. Although the impurities can be removed by appropriate treatments after carbonization, the microstructure of hard carbons can hardly be changed. In this work, taking ficus macrophylla leaves (FMLs) as the model biomass, the effects of impurities and their removing process on the microstructure and Na ion storage performance of hard carbons are investigated. It is found that the presence of Ca and Si-bearing impurities in FMLs results in more graphite-like structure in hard carbons because of their catalytic graphitization effect. The acid and base washing processes after carbonization can mostly get rid of the inorganic impurities is unable to increase the plateau region capacities associating to Na ion insertion in the interlayer of graphitic microcrystals and Na metal filling in micropores. By contrast, by stepwisely removing the Ca and Si-bearing impurities from raw materials before carbonization, hard carbons with high purity, larger interlayer space and more micropores are produced, which exhibit a high reversible specific capacity of 336 mAh g−1 at 20 mA g−1, a high initial Coulombic efficiency of 93 %, excellent rate capability (245 mAh g−1 at 2 A g−1) and robust cycle stability. This study implies that controlling the impurity removal process can simultaneously tune the microstructure of hard carbon anodes derived from biomasses towards high performance Na ion storage.

Cetyl trimethyl ammonium cation expanded NiZn-layered double hydroxide with improved lithium storage property

Exploring new electrode materials with high specific capacity, low cost, and easy preparation is crucial for the development of next-generation lithium-ion batteries (LIBs). Herein, a cetyl trimethyl ammonium cation (CTA+) inserted NiZn-layer double hydroxide (NZH) was prepared by a facile hydrothermal approach. The insertion of CTA+ expands the interlayer distance of NZH from 9.27 to 18.05 Å, accompanied by the formation of a more open nanosheet-like morphology. Particularly, this CTA+ inserted NZH (NZH-C) exhibits a high reversible capacity of 828.8 mA h g−1 after 200 cycles at 0.5 A g−1, far higher than the corresponding capacity (186.2 mA h g−1) of pure NZH; at a relatively high current density of 3.0 A g−1, the NZH-C sample still maintains a reversible capacity of 527.8 mA h g−1. In addition, the NZH-C sample presents an obvious pseudocapacitance effect during the charging and discharging processes; compared with pure NZH, the NZH-C shows a much lower electrochemical reaction resistance, higher lithium diffusivity, and smaller polarization effect. The present work provides a facile and efficient strategy for regulating the interlayer structure and optimizing the lithium storage performance of nickel-based LDH anode materials.

Design and fabrication of reduced graphene oxide (RGO) incorporated NiCo2S4 hybrid composites as electrode materials for high performance supercapacitors

One of the most promising bimetallic sulphides for use in energy-storage systems is NiCo2S4, but further research is required to give it a high reversibility and electrochemical reaction capacity. In this study, we show the rational materials design of an ideal NiCo2S4 nanoparticle as a NiCo2S4/RGO nanocomposite, embedded in a reduced graphene oxide (RGO) matrix. NiCo2S4 nanoparticles, which ranged in size from 20 to 25 nm and were firmly fixed on the surface of RGO sheets, made up the produced composite. As predicted, the produced nanocomposite displayed a high specific surface area, a mesoporous structure, and high conductivity, resulting in a large electroactive area and rapid electron and ion motion. Additionally, we present the advancements in material science, showcasing the NiCo2S4/RGO nanocomposite electrode, which has a long cycle life of 5000 cycles, a high capacitance retention of 85.6 %, and an exceptional specific capacitance of 1505 Fg-1 at 1 Ag-1. A high active-material loading asymmetric supercapacitor serves as an example of the real-world use. The NiCo2S4/RGO nanocomposite exhibits an exceptional 48 Whkg-1 energy density at a power density of 985 Whkg-1, while maintaining a high power density of 7227 Wkg-1 density of 25 Whkg-1. The exceptional stability and electrochemical efficiency of the NiCo2S4/RGO nanocomposite validate that our methodical materials science and technology optimisation in the areas of active substance synthesis, electrode expansion, and device design/fabrication will help advance the development of high-performance supercapacitors in future years.

A Strategy for Anode Recovery and Upgrading by In Situ Growth of Iron-Based Oxides on Microwave-Puffed Graphite.

Faced with the increasing volume of retired lithium-ion batteries (LIBs), recycling and reusing the spent graphite (SG) is of great significance for resource sustainability. Here, a facile method for transforming the SG into a carbon framework as well as loading Fe2O3 to form a composite anode with a sandwich structure is proposed. Taking advantage of the fact that the layer spacing of the spent graphite naturally expands, impurities and intercalants are eliminated through microwave thermal shock to produce microwave-puffed graphite (MPG) with a distinct three-dimensional structure. Based on the mechanism of microwave-induced gasification intercalation, a Fe2O3-MPG intercalation compound (Fe2O3-MPGIC) anode material was constructed by introducing iron precursors between the framework layers and subsequently converting them into Fe2O3 through annealing. The Fe2O3-MPGIC anode exhibits a high reversible capacity of 1000.6 mAh g-1 at 200 mA g-1 after 100 cycles and a good cycling stability of 504.4 mAh g-1 at 2000 mA g-1 after 500 cycles. This work can provide a reference for the feasible recycling of SG and development of high-performance anode materials for LIBs.

Pb/(Ni@RC) composite derived from rice for lead carbon batteries: Excellent conductivity, mass transfer, and reactivity

Enhancing electron/ion transfer and suppressing the hydrogen evolution reaction (HER) represent key objectives in the quest for carbonaceous additives in lead carbon batteries. In this study, we synthesize a porous cellular carbon structure comprising cross-linked nano carbon sheets through a straightforward process involving the expansion and carbonization of rice. Furthermore, by leveraging the distinct reactions of metal oxides and carbon at elevated temperatures, we achieve the simultaneous uniform in-situ loading and embedding of Pb/Ni bimetallic nanoparticles in Pb/(Ni@RC). The etching and embedding of Ni nanoparticles result in remarkable conductivity and the development of an open pore structure. Meanwhile, the incorporation of Pb nanoparticles ensures a low HER rate and a favorable affinity for the anode active material. This positive synergistic mechanism endows Pb/(Ni@RC) with abundant redox-active sites, and mitigates the performance degradation caused by water loss and the disruption of the lead carbon binary phase. Notably, the designed anode demonstrates a high reversible capacity (170 mA h g−1), an exceptionally long cycle life (16830 cycles) under high rate partial state of charge conditions, and an enhanced capacity retention rate (85 %) during partial state of charge operation.

Long-Lifespan Fibrous Aqueous Ni//Bi Battery Enabled by Bi2O3-Bi2S3 Hierarchical Heterostructures.

Bismuth oxide (Bi2O3) materials are considered as great promising anodes for aqueous batteries on account of the high capacity as well as wide potential plateau. Nevertheless, the low conductivity and severe volumetric change of Bi2O3 in the course of cycling are the main limiting factors for their application in energy-storage systems. Herein, we propose and design unique hierarchical heterostructures constructed by Bi2O3 and Bi2S3 nanosheets (NSs) manufactured immediately on the surface of carbon nanotube fibers (CNTFs). The Bi2O3-Bi2S3 (BO-BS) exhibits enhanced conductivity and increased stability in comparison with pure Bi2O3 and Bi2S3. The BO-BS NSs/CNTF electrode indicates exceptional rate capability and cycling stability, while creating a high reversible capacity of 0.68 mAh cm-2 at 4 mA cm-2, as anticipated. Additionally, the quasi-solid-state fibrous aqueous Ni//Bi battery that was built with the BO-BS NSs/CNTF anode delivers an exceptional cycling stability of 52.7% capacity retention after 4000 cycles at 80 mA cm-2, an ultrahigh capacity of 0.35 mAh cm-2 at 4 mA cm-2, and a high energy density of 340.1 mWh cm-3 at 880 mW cm-3. This work demonstrates the potential of constructing hierarchical heterostructures of bismuth-based materials for high-performance aqueous Ni//Bi batteries and other energy-storage devices.

Tube‐in‐Tube Structure Design and In‐situ Growth of Fe3C for Efficient Reaction Kinetics in Lithium‐Sulfur Batteries

AbstractTo improve the sulfur reaction kinetics and inhibit the notorious shuttle effects, a tube‐in‐tube structure decorated by carbon nanotubes (CNT) and Fe3C nanoparticles (TIT/Fe3C‐CNT) is designed as sulfur host for lithium‐sulfur batteries (LSBs) in this work. The construction of tube‐in‐tube structure increases the active sites and the specific surface area of the material. Additionally, Fe3C nanoparticles can effectively adsorb the soluble lithium polysulfides and promote their catalytic conversion, thus greatly alleviating the shuttle effects. As a result of these advantages, the TIT/Fe3C‐CNT‐based cathode exhibits a high reversible capacity of 841 mAh g−1 after 200 cycles with a low decay of 0.056 % per cycle at 0.5 C. This work provides a promising and reasonable approach to the rational design of sulfur host for LSBs.

Optimized Phase and Crystallinity of Cr2(NCN)3 Dominating Electrochemical Lithium Storage Performance.

Cr2(NCN)3 is a potentially high-capacity and fast-charge Li-ion anode owing to its abundant and broad tunnels. However, high intrinsic chemical instability severely restricts its capacity output and electrochemical reversibility. Herein we report an effective crystalline engineering method for optimizing its phase and crystallinity. Systematic studies reveal the relevancy between electrochemical performance and crystalline structure; an optimal Cr2(NCN)3 with high phase purity and uniform crystallinity exhibits a high reversible capacity of 590 mAh g-1 and a stable cycling performance of 478 mAh g-1 after 500 cycles. In-operando heating XRD reveals its high thermodynamical stability over 600 °C, and in-operando electrochemical XRD proves its electrochemical Li storage mechanism, consisting of the primary Li-ion intercalation and subsequent conversion reactions. This study introduces a facile and low-cost method for fabricating high-purity Cr2(NCN)3, and it also confirms that the Li storage of Cr2(NCN)3 can be further improved by tuning its phase and crystallinity.

Long-Cycle Lithium Batteries with LiNi0.8Co0.1Mn0.1O2 Cathodes above 4.5V Enabled by Uniform Coating of Nanosized Garnet Electrolytes

Abstract The pursuit of high-energy cathode materials has been focused on raising the charging cutoff voltage of nickel (Ni)-rich layered oxide cathode such as LiNi0.8Co0.1Mn0.1O2 (NCM811). However, the NCM811 suffers from rapid capacity fading upon cycling at cutoff voltage higher than 4.5 V, owing to their structural degradation and labile surface reactivity. Surface-coating with solid electrolytes has been recognized as an effective method to mitigate the performance failure of NCM811 at high voltage. Herein, the nano-sized Li6.4La3Ta0.6Zr1.4O12 (LLZTO) is uniformly coated on the surface of single-crystal NCM811 particles, accompanied with the long-range Ta5+ diffusion into the transition metal layer of NCM811 lattice. It is revealed that the LLZTO coating can not only inhibit the surface reactions of NCM811 with liquid electrolytes but also play an important role in suppressing the bulk microcracking within the NCM811 particles. The incorporation of Ta5+ ion expands the lattice spacing and thereby improves the homogeneity of the Li+ diffusion in the single-crystal NCM811, which alleviates the mechanical strain and intragranular cracks caused by nonuniform phases-transformation at high charging voltage. The synergy of surface protection and structural stabilization realized by LLZTO coating enables the NCM811-based lithium batteries to achieve a remarkable electrochemical performance. Typically, LLZTO coated NCM811 delivers a high reversible specific capacity of 202.1 mAh⋅g−1 with an excellent capacity retention as high as 70% over 1000 cycles upon charging to 4.5 V at 1 C.

Single Versus Blended Electrolyte Additives: Impact of a Sulfur‐Based Electrolyte Additive on Electrode Cross‐Talk and Electrochemical Performance of LiNiO2||Graphite Cells

AbstractLithium nickel oxide (LNO) is an attractive positive electrode active material for lithium ion batteries (LIBs) due to its high reversible specific capacity and absence of cobalt. Nevertheless, it is prone to structural instabilities that lead to rapid capacity fading, safety concerns and shows in average a lower voltage than mixtures with cobalt, limiting its applicability to date. Herein this study introduces the sulfur‐based electrolyte additive, benzo[d][1,3,2]dioxathiole 2,2‐dioxide (DTDPh), to stabilize the LNO electrode and study its effects on interphase compositions by means of complementary electrochemical and spectroscopic techniques. Obtained results demonstrate an improved galvanostatic cycling performance in terms of cycle life and achievable specific discharge capacity that significantly outperform the common film‐forming additive vinylene carbonate (VC). The cycle life is increased from 102 to 147 cycles compared to the baseline electrolyte and the accumulated discharge energy until end of life is increased by 45%. This study furthermore provides strong evidence of a significant cross‐talk and negative interplay between DTDPh and VC when both are present in the electrolyte formulation. Mechanistic consideration based on density functional theory (DFT) calculations suggest the formation of mobile poly(VC) species, which is supported by the results of post mortem analysis of the resulting interphases.

3D printing of porous hollow nanosphere MoS2@NiS/rGO scaffolds empowering long-cycle sodium-ion batteries

Sodium-ion batteries (SIB), as one of the most appealing electrochemical energy storage devices in the field of energy storage, consistently require optimization for both capacity and long-term cycling performance. The amalgamation of diverse material modification techniques with up-and-coming 3D printing technology presents a promising yet relatively underexplored avenue. Herein, we report a composite material, MoS2@NiS/rGO, as the anode material for SIB, achieving high reversible capacity and outstanding long-term cycling performance, surpassing current reported levels. Through carefully designed anode electrode structure and component interface engineering, the material rate capability (with a capacity of 289.5 mAh g−1 at 0.1 A g−1 and 66.8 mAh g−1 at 5 A g−1) and cycling stability (maintaining a capacity of 131.3 mAh g−1 after 800 cycles at 1 A g−1) are significantly enhanced. The reasons for the improvement in electrochemical performance are elucidated through detailed electrochemical analysis. Encouragingly, we showcase the fabrication of a sodium-ion full battery entirely through 3D printing (3DP), achieving an area loading capacity as high as 8.23 mg cm−2 and retaining a capacity of 82.1 mAh g−1 after 240 cycles at 0.1 A g−1. This work underscores the pivotal significance of 3D-printed sodium-ion batteries in advancing the frontier of energy storage technology.

Binder-Free Anodes for Potassium-ion Batteries Comprising Antimony Nanoparticles on Carbon Nanotubes Obtained Using Electrophoretic Deposition.

Antimony has a high theoretical capacity and suitable alloying/dealloying potentials to make it a future anode for potassium-ion batteries (PIBs); however, substantial volumetric changes, severe pulverization, and active mass delamination from the Cu foil during potassiation/depotassiation need to be overcome. Herein, we present the use of electrophoretic deposition (EPD) to fabricate binder-free electrodes consisting of Sb nanoparticles (NPs) embedded in interconnected multiwalled carbon nanotubes (MWCNTs). The anode architecture allows volume changes to be accommodated and prevents Sb delamination within the binder-free electrodes. The Sb mass ratio of the Sb/CNT nanocomposites was varied, with the optimized Sb/CNT nanocomposite delivering a high reversible capacity of 341.30 mA h g-1 (∼90% of the initial charge capacity) after 300 cycles at C/5 and 185.69 mA h g-1 after 300 cycles at 1C. Postcycling investigations reveal that the stable performance is due to the unique Sb/CNT nanocomposite structure, which can be retained over extended cycling, protecting Sb NPs from volume changes and retaining the integrity of the electrode. Our findings not only suggest a facile fabrication method for high-performance alloy-based anodes in PIBs but also encourage the development of alloying-based anodes for next-generation PIBs.

Engineering FeSe2 encapsulated within carboxymethylcellulose-derived porous carbon for enhanced surface reaction kinetics in Li-ion half/full battery anodes

Encapsulation of transitional metal selenides within the porous nanocarbon network has been regarded as a highly advantageous strategy for improving anode performance in terms of capacity, cycle-to-cycle stability, and operational durability for Li+ storage. Herein, a mildly sol-gel process and in-situ self-transformation strategy were employed to fabricate FeSe2 encapsulated within eco-friendly carboxymethylcellulose (CMC)-derived porous carbon, achieving a feasible capacity and relatively durable structure. The FeSe2@PC anode with square-built Li+/e− diffusion pathway exhibits a comparatively high reversible capacity of up to 758 mAh g−1 at 0.1 A g−1 and relatively good cycling stability, with a capacity retention of 83% after 500 cycles at 1 A g−1 in half cells. Furthermore, FeSe2@PC//LiMn2O4 full cells also demonstrate relatively outstanding electrochemical performance when paired with a LiMn2O4 cathode. The nanoconfinement electrode configuration, featuring interconnected external/internal carbon shell/FeSe2 nanoparticles, not only provides good electrical conductivity and buffering capacity for volume changes but also facilitates electrolyte infiltration and surface/near-surface interactions between electroactive FeSe2 and Li+. Kinetic analysis through cyclic voltammetry, galvanostatic intermittent titration technique, and electrochemical impedance spectroscopy indicates exceptional Li+/e− transport kinetics. Employing green and eco-friendly materials in energy storage is crucial for advancing sustainable energy technologies, and the engineered FeSe2@PC nanocomposite demonstrated in this study offers promising potential towards this objective.

Boosting sodium storage performance of biomass-derived porous carbon anodes by surface functionalized strategy

In order to enhance the sodium ion storage performance of biomass-derived carbon anode materials, a surface functionalization strategy was employed through a simple acid etching method on porous carbon. The resulting functionalized carbon exhibits a hierarchically porous structure, expanded interlayer spacing, and oxygen-containing functional groups. The redox reactions occurring at the surface between Na ions and carbonyl groups provide additional sites for sodium ion storage, thereby improving cycling capacity and rate capability. Theoretical calculations and electrochemical tests further demonstrate that the functionalized carbon can increase the surface-controlled sodium storage capacity by modifying the transport and adsorption processes of sodium ions. After 200 cycles at a current density of 100 mA g−1, the carbon anode, which was surface-functionalized with an etching time of 6 h, achieve a high reversible capacity of 273 mA h g−1. Furthermore, it displays improved rate performance with a capacity of 194 mA h g−1 at a high current density of 2 A g−1 for sodium-ion batteries. This study introduces an effective and general strategy for the cost-effective and large-scale synthesis of carbon anode materials for sodium-ion batteries.

Water-in-Salt Gel Biopolymer Electrolytes for Flexible and Wearable Zn/Alkali Metal Dual-Ion Batteries.

Zn/alkali metal dual-ion batteries (ZM DIBs) with highly concentrated water-in-salt (WiS) electrolytes are promising next-generation energy storage systems. This enhanced design of Zn-ion rechargeable batteries offers intrinsic safety, high operating voltage, satisfactory capacity, and outstanding cyclic stability. Herein, taking the concept of highly concentrated electrolytes one step further, we introduce water-in-salt gel biopolymer electrolytes (WiS-GBEs) by encapsulating Zn/Li or Zn/Na bisalt compositions in a cellulose membrane. WiS-GBEs inherit the electrochemical merits of highly concentrated electrolytes (i.e., wide voltage window, high ionic conductivity, etc.) and excellent durability of gel biopolymer structures. Both types of WiS-GBEs apply to coin- and pouch-cell compartments of ZM DIBs, offering a high plateau voltage (>1.8 V vs. Zn2+/Zn), good and reversible capacity (118 and 57 mAh g-1 for Zn/Li and Zn/Na cells, respectively), and outstanding cycling stability (more than 90% after 1,000 cycles). Essentially, the pouch cells with WiS-GBEs present superior durability, flexibility, and capacity endurance under various bending stress conditions (90% capacity retention under 0-180° bending modes), indicating their potential capability to power wearable electronics. The practical powering ability of Li- and Na-based pouch systems is demonstrated by the example of a wearable digital timer.

S-doped MXene@porous carbon nano-fiber composite for improved sodium storage performance

Sodium-ion batteries have attracted considerable interest of many scholars due to their low cost and similar energy storage mechanism to lithium-ion batteries. Considering the poor electrochemical redox reaction kinetics and low structural stability resulting from the larger radius of Na+ (0.102 nm), we have elaborately designed novel sulfur-doped MXene/porous carbon nano-fiber composites (S-MX@CNF) as anodes for SIBs via a synergistic assembly and sulfidation treatment approach. The S-MX@CNF composites have a multi-layered structure, which not only prevents restacking of MXene layers and increases accessible active sites, but also enhances the overall electrode conductivity. The composites exhibit a unique interconnected conductive network frame structure and increased interlayer spacing, which facilitates fast ionic and electronic transport rates. Additionally, the robust composites exhibit high chemical stability, enabling it to tolerate volume changes during the rapid charge/discharge process. As a result of these synergistic effects, the S-MX@CNF displays a high reversible capacity of 304 mAh/g (0.5 A/g) after 1000 cycles and long cycle stability of 170 mAh/g (3 A/g) with only 0.1 % degradation per cycle within 4900 cycles. This work opens up new opportunities for further advances in synergistic assembly and heteroatom doping strategies for composites in energy storage devices.