Rechargeable magnesium-ion batteries (RMBs) demonstrate notable benefits, including higher theoretical energy density, cost-effectiveness, and improved safety characteristics, positioning them as a viable substitute for conventional energy storage solutions. Nevertheless, the ongoing development of high-performance RMBs continues to face inevitable challenges, such as unsatisfactory practical capacity, inadequate cycle durability, swift energy degradation, and a comparatively limited-service life. Herein, CoS/NiS nanomaterials with cubic-shaped morphology were prepared by a two-step metal sulfide template-free solvothermal synthesis method. The material with internal cavity structure effectively mitigates the large expansion of magnesium-ion battery cathode material due to Mg2+ embedding during the charging and discharging process, and provides a robustness electrode-electrolyte interface, thus greatly improving the cycle life. Besides, the introduction of Ni elements into CoS materials may form heterojunctions thereby lowering the potential barrier of the conversion reaction and improving the reaction kinetics and redox reversibility. In addition, the abundance of highly electronegative SS bonds in the CoS/NiS material, which also provides many electrochemically active sites and smooth transport paths for the embedding of Mg2+, leads to the reduction of its polarization and the improvement of its reaction kinetics, which makes the CoS/NiS as a RMBs cathode material with a high specific capacity and a long cycling life. Thus, this research presents a feasible and effective strategy for enhancing the Mg2+ storage capability of engineered CoS nanomaterials, with potential applicability and adaptability to other electrode materials.

The Li-rich manganese-based oxides (LRMO) with high operating voltage and large reversible capacities can demonstrate comprehensive advantages of intrinsic safety and high energy density when employed in all-solid-state lithium batteries (ASSLBs). However, severe interfacial incompatibility with solid electrolytes (SEs) arising from unstable lattice oxygen and sluggish Li+ ionic transport hinders their practical application. In this contribution, the gradient-modified structure containing S, Zr co-doping near-surface and amorphous Zr(SO4)2 coating is simultaneously established onto LRMO cathode by a one-step mechano-fusion process. The synergistic co-functionalization stabilizes the oxygen framework, enhances charge transport, and suppresses oxygen dimerization under high potential. Besides, the amorphous Zr(SO4)2 coating evenly adhering onto LRMO bulk ensures long-term intimate contact with SEs to guarantee electrochemical activities and restrains interfacial parasitic reactions. Consequently, the optimized A-LRMO cathode exhibits a high discharge capacity of 292 mAh/g at 0.1 C and 81.8% capacity retention after 2000 cycles at 1 C. Pouch cells delivered an areal capacity of 8.5 mAh/cm2 with >99.6% Coulombic efficiency. This gradient-modification strategy offers an effective pathway to improve interfacial stability and accelerate the practical application of LRMO-based ASSLBs.

The electrochemical performance of all-solid-state lithium batteries (ASSLBs) can be markedly enhanced by resolving issues arising from cathode conductive additives (CCAs), including excessively high interfacial impedance, inadequate compatibility with solid electrolytes, and insufficient adaptability to the composite cathode. Here, the embedding of ultra-thin and ultra-stable MoS0.25Se1.75 nanosheets onto a vapor-grown carbon fibers (VGCF) substrate are successfully fabricated (MoS0.25Se1.75@VGCF) as CCAs within a LiCoO2-based composite cathode for Li6PS5Cl (LPSC)-based ASSLBs. This advanced nanostructure design not only effectively suppresses the presence of hydroxyl groups (-OH) on the surface but also induces a synergistic effect that builds up a strong internal electric field and simultaneously lowers the Li+ ions migration energy barrier, which can mitigate the occurrence of LPSC degradation at the CCAs|LPSC interface while establishing dual electron/Li+ ion transport pathway, thus strengthening the compatibility of composites cathode interfaces for the improvement of electrochemical performance. Consequently, the assembled LCO|MoS0.25Se1.75@VGCF|LPSC-based ASSLBs exhibit exceptional performance, demonstrating a high discharge capacity of 131.24 mAh & sdot;g-1 at 0.1C, a high coulombic efficiency of 92.34 %, and an excellent capacity retention of 90.41 % after 1000 cycles at 0.5C. This finding introduces a novel synergistic strategy, which offers a fresh approach to mitigate interfacial instability in composite cathodes, thereby further facilitating the commercialization of ASSLBs.

The architecture of high-efficiency and long-term seawater-splitting electrocatalysts capable of suppressing the undesirable chloride electrochemistry and corrosion is paramount for seawater electrolysis technology. Herein, a bifunctional electrocatalyst composed of Ni,Cd-codoped iron vanadate supported on nickel foam (denoted as Ni,Cd-Fe2VO4/NF) is rationally designed. The triggered synergistic effect of Ni,Cd co-doping can modulate the electron configuration of Fe2VO4, which not only optimizes the adsorption energy of reactants and intermediates and simultaneously strengthens the electron transfer ability, but also stabilizes the Fe/V sites with high valence in Fe2VO4, which preferentially adsorbs H2O and OH- while electrostatically repelling Cl- during the seawater electrolysis. Consequently, the Ni,Cd-Fe2VO4/NF electrocatalyst only requires extremely low overpotentials of 236 and 254 mV for OER and HER to reach a current density of 500 mA cm-2 in 1 m KOH + seawater, respectively. And it also maintains stable operation for 200 h with negligible performance attenuation. Notably, the zero-gap electrolyzer assembled with Ni,Cd-Fe2VO4/NF electrocatalysts exhibits an ultralow voltage of 1.74 V at a current density of 500 mA cm-2 in 1 m KOH + seawater, accompanying an ultra-long lifespan of 3000 h without significant performance degradation, underscoring its great potential for large-scale practical application.

Rechargeable magnesium batteries (RMBs) possess the merits of greater theoretical capacity, cheaper magnesium metal and not easily producing branched crystals, and greater safety. Therefore, the current researches mainly concentrate on the exploration of high-performance RMBs in the initial stage, but still face many gigantic challenges. Herein, petal-shaped nanorods CoS/CuS materials are successfully synthesized as RMBs cathode materials through a two-step metal sulfide template-free solvent-thermal synthesis method, which can effectively improve the reaction kinetics due to the petal-like nano-structure and provide rich electrochemically active sites to decrease the transport barrier of Mg2+, thus contributing to the enhancement of the reaction kinetics of magnesium storage in RMBs. The electrochemical performance test illustrates that CoS/CuS composite nanomaterials can considerably improve the charging and discharging specific capacity of the batteries as well as the voltage of the batteries due to the existing synergistic effect between them. The specific capacity of CoS/CuS cathode still can still be maintained as high as 62.8 mAh g-1 after 300 cycles at 200 mA g-1 . And the specific capacity of this electrode material changes from 180.6 mAh g-1 to 30 mAh g-1 at the current densities from 100 mA g-1 to 1000 mA g-1 , and when the current density is restored to 100 mA g-1 , the specific capacity gradually recovered to 178.6 mAh g-1 , which showed better rate performance and ultra-high cycling stability. This work highlights how the introduction of CuS into CoS nanostructures can benefit the reversibility and cyclicity of the magnesium storage reaction and offers an original and practical route for the modification of RMBs electrode materials with good electrochemical properties. (c) 2025 Institute of Process Engineering, Chinese Academy of Sciences. Publishing services by Elsevier B.V. on behalf of KeAi Communications Co. Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).

The design of high-performance bifunctional electrocatalysts is critical for H2 generation through electrochemical water electrolysis. Here, the Ni heteroatoms-decorated Co@Co2Mo3O8 heterojunctions hybridized with rape pollen (RP)-derived nitrogen-doped porous carbon frameworks (Ni-Co@Co2Mo3O8/CNPs) were innovatively fabricated by wet-impregnation treatment and thermal annealing. This designed nanostructure can provide effective electronic promoters and innumerable heterointerface sites while simultaneously enabling extremely strong interactions among these components, not only reinforcing the nano-structural durability and facilitating the interfacial electron transformation, but also arousing the synergistic effect to actuate the rearrangement of electron configuration and ameliorate the adsorption capacity of intermediates, ultimately achieving comprehensive enhancement of electrocatalytic performance. On these grounds, a fine-tuned Ni-Co@Co2Mo3O8/CNPs possesses the excellent electrocatalytic performance, featuring ultra-low overpotentials of 49 and 194 mV HER and OER at 10 mA cm- 2 respectively. Meantime, when Ni-Co@Co2Mo3O8/CNPs is applied in an H-type electrolyzer, it can obtain an exceptionally low voltage of 1.45 V at 10 mA cm- 2, coupled with remarkable durability of 200 h. In a zero-gap alkaline electrolyzer, it can achieve an ultra-low voltage of 1.80 V at 500 mA cm- 2, accompanied by an ultra-long operational lifespan of 2500 h.

Platinum loading is a critical factor limiting the large-scale application and commercial deployment of proton exchange membrane fuel cells (PEMFCs). Accelerated stress testing (AST) is widely adopted to evaluate the durability of PEMFCs. In this study, a five-cell PEMFC stack was assembled and subjected to a 210-hour AST protocol. Polarization curves, electrochemical impedance spectroscopy (EIS), and distribution of relaxation times (DRT) analysis were employed to assess stack performance and identify potential decay patterns across individual cells. Post-test, samples were extracted along the cathode reactant flow path from each cell and reassembled into single-cell configurations for localized degradation analysis. Results reveal that cells with higher platinum loading experienced more severe performance degradation. The extent of performance loss and catalytic surface deterioration exhibited a strong dependence on platinum loading levels. In high-platinum-loading cells, the primary degradation mechanism was identified as reactant transport obstruction due to particle agglomeration. In contrast, medium-platinum-loading cells showed negligible membrane electrode assembly (MEA) structural deterioration but significant platinum migration, as confirmed by elemental analysis. Conversely, low-platinum-loading cells suffered substantial catalyst layer degradation, attributable to insufficient catalyst coverage. This study underscores the importance of balancing platinum loading with the multi-scale performance requirements of PEMFCs, such as lifespan and efficiency, providing valuable insights for future stack design and optimization.

Exceptional electrochemical performances of all-solid-state lithium metal batteries (ASSLMBs) can be achieved by effectively inhibiting damaging of reactive oxygen species (ROSs) formed by oxidation of the inevitably present surface groups on the carbon-based conductive agents (CCAs) and upon charging transition metal oxide based cathodes. Herein, we report on the use of highly effective novel CCA additive based on biomass-derived carbonaceous nanomaterials produced from carbonized pollen uniformly coated by nano MoO2 through a bio-templating method (CP@MoO2) in composite high energy cathodes of ASSLMBs. The rational design of this porous nano-composite additive not only makes it difficult for oxygen-containing functional groups to survive on the surface, but also promotes electrocatalytic adsorption and transformation of ROSs within composite cathodes, thus avoiding their detrimental effects. And rapid and homogeneous conductions of Li+/e(-) within the composite cathodes are ensured thanks to the use of the CP@MoO2 additive. As a result, ASSLMBs employing typical LiCoO2 and promising Li-rich Mn-based oxide cathodes could demonstrate excellent cycling stability retaining 99.9 % of discharge capacity after 500 cycles at 0.2C and display capacity retention of over 87 % after 3000 cycles at 5C with a steady average coulombic efficiency (>99.98 %).

Rechargeable magnesium-ion batteries (RMBs) exhibit distinct advantages, such as superior theoretical capacity, economic viability, and enhanced safety features, making them a promising alternative to traditional energy storage systems. Nevertheless, the current research of high-performance RMBs is still fraught with many shortcomings of the unexpected actual capacity, poor cycling stability rapid energy decay, and a relatively short lifespan. Herein, Grape-bunch CoS/Te materials are prepared by one-step metal sulfide template-free anion-doped solvent-thermal synthesis. The as-prepared material displays a well-defined skeletal structure, which maximizes electrolyte-electrode interaction and shortens Mg2+ migration pathways. Besides, the CoS/Te composites exhibit lattice expansion because of anionic TeO32- doping manifested as widening of the lattice spacing, which significantly reduces the resistance to the interlayer movement of Mg2+, thus contributing to improvement of the reaction kinetics of magnesium storage in RMBs. The anion-doped CoS-based composites not only weaken Mg2+-cathode electrostatic interactions but also provide numerous active sites, accelerating magnesium storage kinetics. The conversion reaction energy barrier is significantly reduced through Te incorporation in CoS, with reaction kinetics being simultaneously optimized, which contributes to enhanced capacity retention, superior rate performance, and prolonged cycling stability. The electrochemical storage mechanism of converted Mg2+ was revealed by characterization. Therefore, this study offers a practical and viable approach for elevating the Mg2+ storage performance of modified CoS nanomaterials, which is expected to be applicable and generalizable to other electrode materials.

All-solid-state lithium batteries (ASSLBs) are considered one of the most promising candidates for future energy storage devices. Among them, sulfide-based solid electrolytes (SSEs) have garnered extensive research attention due to their outstanding thermal stability, high ionic conductivity, low Young's modulus, and wide electrochemical window. In order to improve the rate performance, cycle stability and capacity of ASSLBs, people usually use SSEs, conductive carbon, together with active materials (AMs) to construct composite cathodes. Despite some notable progress in research related to composite cathodes, interface issues have consistently posed obstacles to their industrialization and commercialization. This article comprehensively summarizes the influence of the structure, morphology, composition, and preparation process of composite cathodes on interface issues, with special emphasis on modification strategies to solve the interface problems. This article points out several promising research directions that may solve the interface issues and offer some insights and guidance to researchers in the related fields.

Solid-state lithium metal batteries are one of the most promising options for next-generation batteries pursuing high-energy density and high-safety. However, the inevitable volatilization of lithium compounds during sintering leads to low relative density and low ionic conductivity of solid-state electrolytes. Herein, the dynamic lithium-compensation mechanism is proposed to facilitate the densification of Ta-substituted garnet-type electrolyte (Li6.5La3Zr1.5Ta0.5O12 (LLZT)) through the reversible manipulating of Li2O atmosphere. Li2ZrO3 is used as mother powder additive, which reacts with Li2O in sintering atmosphere and forms Li6Zr2O7. Li2ZrO3/Li6Zr2O7 buffer pair manipulates the sintering Li2O atmosphere, which is vital for LLZT, within the Li2O partial pressure range corresponding to Li2ZrO3 and Li6Zr2O7. Furthermore, the reversibility mechanism of buffer pair for Li2O absorption and release is revealed. The obtained LLZT exhibits a relative density of over 96

Rechargeable Magnesium ion batteries (RMBs) are investigated as lithium-ion batteries (LIBs) alternatives owing to their favorable merits of high energy density, abundance and low expenditure of Mg, as well as especially non-toxic safety and low risk of dendrite formation in anodes, which endows them to be more easily assembled in electric-power vehicles for the extended application of civilian-military fields. Nevertheless, the high charge density, strong polarization effect, and slow diffusion kinetics of Mg2+ remain a large obstacle and thus enormous efforts have to be paid to mend the gap with commercial demand for cathode materials. At present, RMBs cathode materials mainly contain transition metal sulfides/oxides, polyanionic compounds and Prussian blue analogs, and several methods such as nano structuring, doping regulation and coating modification have been applied to materials design for better performance. In this paper, the current research status of RMBs cathode materials at home & abroad is arranged and summarized along with challenges of development in the future focusing on synthesis of RMBs cathode materials with high energy density as well as satisfactory cycling performance. And this analysis aims to provide reference and basis for researchers working on RMBs technology advancement.

Sodium-ion batteries (SIBs) are investigated as promising alternatives to lithium-ion batteries (LIBs) on account of the economical abundance and reliable availability of sodium, as well as its analogous chemical properties compared to lithium. Nevertheless, the performance of SIBs is severely restricted by the availability of satisfactory cathode nanomaterials with stable frameworks to accommodate the transportation of large-sized Na+ ions. These challenges can be effectively resolved when exploiting Prussian blue (PB) and its analogs (PBAs) as SIB cathodes. This is mainly because PB and PBAs have 3D open frameworks with large interstitial space, which are more favorable for fast insertion/extraction of Na+ ions during the charging/discharging process, thus enabling the improvement of integrated performance in SIB systems. This overview offers a comprehensive summarization of recent advancements in the electrochemical performance of PB and PBAs when employing them as cathodes in SIBs. For better understanding, the fabrication strategy, structural characterization, and electrochemical performance exposition are systematically organized and explained according to tuning PB and metal-based PBAs. Additionally, the current trajectories and prospective future directions pertaining to the utilization of PB and PBA cathodes in the SIB system are thoroughly examined and deliberated upon.

Li10.35Ge1.35P1.65S12 (LGPS) electrolyte has garnered attention due to its high ionic conductivity and processability. However, its strong incompatibility with lithium metal hinders its practical application. Conventional interlayer strategy isolates Li from LGPS, avoiding the detrimental side reactions, but lithium dendrite penetration is still a problem. To address the aforementioned challenges, we develop a PVDF-HFP-supported PDOL-based interlayer (PDOL/PVDF-HFP), which stabilizes the LGPS/Li interface by synergistically physically inhibiting and chemically scavenging lithium dendrites. The multifunctional feature of the interlayer comes from the use of a bifunctional initiator, InCl3. On the one hand, InCl3 induces the polymerization of DOL, forming a physical separator and protecting lithium from LGPS; on the other hand, in situ reactions between In3+/Cl- and Li form a LiCl/LiF/LiIn hybrid SEI, homogenizing the surface Li+ flux and suppressing lithium dendrite formation and penetration. In addition, an unexpected dynamic microdendrite scavenging is realized by virtue of the side reactions of LGPS/Li, which converts the undesirable reaction to be an advantage in our design. Benefiting from the comprehensive advantages of such design, the constructed sulfide-based solid-state batteries achieve a super low interfacial impedance of 5.1 Ω, a high critical current density (CCD) value over 5 mA/cm2, and a super long cycling stability over 8000 h. Our synergistic interlayer strategy would open an effective avenue for solving interfacial challenges for practical sulfide-based solid-state batteries.

The electrochemical performance of all-solid-state lithium batteries (ASSLBs) can be significantly improved by addressing the challenges posed by space charge layer (SCL) effect, which plays a crucial role in determining Li+ ions transport kinetic at cathodic interface. Therefore, it is critical to realize the in situ inspection and visualization of SCL behaviors for solving sluggish Li+ ions transport issues, despite remaining grant challenges. Therewith, the well-defined model of LiNbO3-coated NCM (NCM@LNO) cathode is constructed and assembled for the representative Li6PS5Cl-based ASSLBs, which not only ensures excellent cathodic compatibility, but also preferably enables the better monitoring of Li+ ions transport kinetics. Combining ex situ analysis with DFT calculation, the formation and evolution mechanism of SCL are comprehensively understood, and the relationship between well-controlled SCL configuration and Li+ electrochemical behavior has been also further illustrated and established through the operando Raman spectroscopy. On these grounds, the preferred NCM@LNO cathodes acquire the enhanced discharge capacity of 90.6% (144.8 mAh g(-1)) after 100 cycles and it can still deliver the exceptional capacity of 136.2 mAh g(-1) after 800 cycles in ASSLBs. Hence, the research will pave up a new perspective for fundamental scientific insight of the SCL and reasonable tailoring of cathodic interface for high-efficiency ASSLBs.

Rechargeable magnesium batteries (RMBs) are cost-effective and dendrite-free, making them desirable for largescale applications. Nevertheless, the exploration of high-performance cathodes still remains a great challenge in magnesium battery research. Herein, the CoSe porous polyhedra induced by Te heteroatoms (CoSe/Te) are successfully prepared by two-step metal-organic framework (MOF)-template assisted method and investigated as high-efficiency cathodes for rechargeable MIBs. In this regard, the affluent porous structure can facilitate the transport of Mg2+ ions while the introduction of Te heteroatoms can reduce the conversion reaction barrier, boost the kinetics and redox reversibility and excite the electron conduction to build active nanostructured domains for highly reversible Mg storage reactions. As a consequence, the CoSe/Te maintains the high specific capacity of 150.6 mAh g-1 after 600 cycles at 200 mA g-1, with a superior capacity retention rate of 75.3%. Moreover, the specific capacity of such electrode materials changed from 260 mAh g-1 to 41 mAh g-1 when the current density increased from 100 mA g-1 to 2000 mA g-1, and gradually recovered to 256.5 mAh g-1 when the current density returned to 100 mAh g-1, exhibiting a better rate performance. This work highlights how micronanostructures can favor magnesium storage reaction reversibility and cyclability and also provide insights into rational electrode design for storing magnesium cations in future studies.

The electrochemical performance of all-solid-state Li metal batteries (ASSLMBs) can be improved by resolving the challenges triggered by the uncontrolled growth of Li dendrites throughout the solid electrolytes (SEs). Herein, a well-defined composite of micro-Li6PS5Cl (LPSC) and nano-Li1.3Al0.3Ti1.7(PO4)(3) (LATP) is designed as a LPSC-LATP interlayer sandwiched between LPSC electrolytes for ASSLMBs. This fabrication exhibits electron-blocking functionalities, which reduce the probability of reaction with Li+ ions for the formation of anode-initiated and grain boundary (GB)-initiated dendrites. More importantly, it also creates localized eliminated micro-environments of Li dendrites through the high transient reactivity between them, and the remaining cracks can be dynamically and effectively filled by decomposition products, thereby clearly suppressing Li dendrite nucleation, propagation and penetration as well as simultaneously contributing to the enhancement of battery performance and stability. With this approach, a fine-tuned LPSC-LATP (8S-2O) interlayer enables symmetrical Li/LPSC/8S-2O/LPSC/Li cells to achieve an ultra-high critical current density (CCD) of over 5 mA cm(-2) at room temperature, and ultra-long-term cycling at a current density of 10 mA cm(-2) for over 1600 h. Additionally, ASSLMBs employing commercial LiCoO2 cathodes can deliver exceptional durability, with an extremely high 85.6% retention of initial discharge capacity and coulombic efficiency (CE) of >99.6% after 1200 cycles at 1C (1.28 mA cm(-2)). These experimental batteries demonstrate the application potential of this configuration of SEs for the commercialization of ASSLMBs.

CO2 reduction plays a vital role in carbon capture, utilization and storage (CCUS), whereas electroreduction method has attracted considerable attention because of its high selectivity, safety, and energy efficiency. Solid oxide electrolysis cells (SOECs) have exhibited significant advantages in CO2 reduction and utilization. Among all the components of SOEC, the cathode materials are crucial due to the complex mechanism and harsh working conditions at the cathode. Perovskite oxide-based cathodes show great prospect for CO2 conversion with excellent catalytic activity, redox stability, and coking resistance compared to conventional cermet cathodes. This review mainly summaries the recent research progress on the CO2 reduction mechanism and the electrochemical performance of various perovskite cathodes. The effect of different modification methods on the performance of perovskite cathodes is explored, and the possible solutions to degradation are discussed. The common problems of perovskite cathodes and improving methods are also suggested in this review.

Lithium metal batteries based on metallic Li anodes have been recognized as competitive substitutes for current energy storage technologies due to their exceptional advantage in energy density. Nevertheless, their practical applications are greatly hindered by the safety concerns caused by lithium dendrites. Herein, we fabricate an artificial solid electrolyte interface (SEI) via a simple replacement reaction for the lithium anode (designated as LNA-Li) and demonstrate its effectiveness in suppressing the formation of lithium dendrites. The SEI is composed of LiF and nano-Ag. The former can facilitate the horizontal deposition of Li, while the latter can guide the uniform and dense lithium deposition. Benefiting from the synergetic effect of LiF and Ag, the LNA-Li anode exhibits excellent stability during long-term cycling. For example, the LNA-Li//LNA-Li symmetric cell can cycle stably for 1300 and 600 h at the current densities of 1 and 10 mA cm-2, respectively. Impressively, when matching with LiFePO4, the full cells can steadily cycle for 1000 times without obvious capacity attenuation. In addition, the modified LNA-Li anode coupled with the NCM cathode also exhibits good cycling performance.

Alloying-based material has achieved tremendous appealing being anode used in sodium-ion batteries (SIBs) by virtue of its relatively giant sodium storage specific capacity along with low discharge platforms. Nevertheless, the sluggish ion transmission dynamics and the huge volume change during cycling induced irreparable particle pulverization and agglomeration result in collapse of electrode structure and deterioration of cycling properties. In this work, three-dimensional cross-linked carbon nanotube-interspersed SnSb@CNF integrated structure (SnSb@CNF/CNT) is designed and synthesized. In this ingenious nanostructure, CNTs interspersed between CNF frames play the role of electron transport and diffusion "bridges" for enhancing the electrical conductivity of anode materials and relieve aggregation of SnSb alloy particles, the N doped-CNFs serve as external frame could efficiently mitigate dramatic volume effect to maintain system integrity. Based on these constructive advantages, the elastic conductive system can be directly available as anode for SIBs, showing ultralong cycling performance of 210 mAh g-1 over 700 sodiation/desodiation processes with a current density of 0.5 A g-1, even 161 mAh g-1 following 1000 cycling under a high current density of 1 A g-1 accompanied by an almost 100% superb capacity retention ratio, as well as distinguished high rate performance (470 mAh g-1 with a returned current density of 0.05 A g-1). This work shed distinctive insight to construct in situ three-dimensional cross-linked freestanding alloying-based anode materials used in alternative electrochemical grid-scale application.