Advanced rechargeable lithium-ion batteries based on bendable ZnCo2O4-urchins-on-carbon-fibers electrodes

A novel class of ZnCo₂O₄-urchins-on-carbon-fibers matrix has been designed, characterized, and used to fabricate high-performance energy storage devices. We obtained a reversible lithium storage capacity of 1180 mA·h/g even after 100 cycles, demonstrating the highreversible capacity and excellent cycle life of the as-prepared samples. Tested as fast-charging batteries, these electrodes exhibited a considerable capacity of 750 mA·h/g at an exceptionally high rate of 20 C (18 A/g), with an excellent cycle life (as long as 100 cycles), which are the best high-rate results reported at such a high charge/discharge current density for ZnCo₂O₄-based anode materials in lithium rechargeable batteries. Such attractive properties may be attributed to the unique structure of the binder-free ZnCo₂O₄-urchins-on-carbon-fibers matrix. Full batteries were also developed by combining the ZnCo₂O₄ anodes with commercial LiCoO₂ cathodes, which showed flexible/wearable and stable features for use as very promising future energy storage units.      

Molten-salt chemical exfoliation process for preparing two-dimensional mesoporous Si nanosheets as high-rate Li-storage anode

Two-dimensional (2D) materials have attracted enormous attention due to their functional applications in energy storage. In this work, a low-temperature molten-salt chemical exfoliation methodology is developed for producing free-standing 2D mesoporous Si through deintercalation of CaSi₂ in excess molten AlCl₃ at 195 °C. The average dimension of these sheets is 1.5 μm, and the thickness of a single sheet is approximately 10 nm. The as-prepared 2D Si has a Brunauer–Emmett–Teller surface area of 154 m²·g^?1 and an average pore size of 5.87 nm. With this unique structure, the 2D Si exhibits superior Li-storage performance, including a reversible capacity of 2,974 mA·h·g^?1 at 0.2 C, reversible capacities of 2,162, 1,947, and 1,527 mA·h·g^?1 at 0.8, 2, and 5 C after 200 cycles, and a capacity retention of 357 mA·h·g^?1 even at 30 C (90 A·g^?1).

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NiaSi2O5（OH）4 Multi-Walled Nanotubes with Tunable Magnetic Properties and Their Application as Anode Materials for Lithium Batteries

Highly crystalline and thermally stable pure multi-walled Ni₃Si₂O₅(OH)₄ nanotubes with a layered structure have been synthesized in water at a relatively low temperature of 200–210 °C using a facile and simple method. The nickel ions between the layers could be reduced in situ to form size-tunable Ni nanocrystals, which endowed these nanotubes with tunable magnetic properties. Additionally, when used as the anode material in a lithium ion battery, the layered structure of the Ni₃Si₂O₅(OH)₄ nanotubes provided favorable transport kinetics for lithium ions and the discharge capacity reached 226.7 mA·h·g⁻¹ after 21 cycles at a rate of 20 mA·g⁻¹. Furthermore, after the nanotubes were calcined (600 °C, 4 h) or reduced (180 °C, 10 h), the corresponding discharge capacities increased to 277.2 mA·h·g⁻¹ and 308.5 mA·h·g⁻¹, respectively.      

Hydrogenated vanadium oxides as an advanced anode material in lithium ion batteries

Current research on vanadium oxides in lithium ion batteries (LIBs) considers them as cathode materials, whereas they are rarely studied for use as anodes in LIBs because of their low electrical conductivity and rapid capacity fading. In this work, hydrogenated vanadium oxide nanoneedles were prepared and incorporated into freeze-dried graphene foam. The hydrogenated vanadium oxides show greatly improved charge-transfer kinetics, which lead to excellent electrochemical properties. When tested as anode materials (0.005–3.0 V vs. Li/Li⁺) in LIBs, the sample activated at 600 °C exhibits high specific capacity (～941 mA·h·g^?1 at 100 mA·g^?1) and high-rate capability (～504 mA·h·g^?1 at 5 A·g^?1), as well as excellent cycling performance (～285 mA·h·g^?1 in the 1,000^th cycle at 5 A·g^?1). These results demonstrate the promising application of vanadium oxides as anodes in LIBs.

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Self-standing Na-storage anode of Fe<Subscript>2</Subscript>O<Subscript>3</Subscript> nanodots encapsulated in porous N-doped carbon nanofibers with ultra-high cyclic stability

Ultrasmall γ-Fe₂O₃ nanodots (～ 3.4 nm) were homogeneously encapsulated in interlinked porous N-doped carbon nanofibers (labeled as Fe₂O₃@C) at a considerable loading (～ 51 wt.%) via an electrospinning technique. Moreover, the size and content of Fe₂O₃ could be controlled by adjusting the synthesis conditions. The obtained Fe₂O₃@C that functioned as a self-standing membrane was used directly as a binder- and current collector-free anode for sodium-ion batteries, displaying fascinating electrochemical performance in terms of the exceptional rate capability (529 mA·h·g^–1 at 100 mA·g^–1 compared with 215 mA·h·g^–1 at 10,000 mA·g^–1) and unprecedented cyclic stability (98.3% capacity retention over 1,000 cycles). Furthermore, the Na-ion full cell constructed with the Fe₂O₃@C anode and a P2-Na_2/3Ni_1/3Mn_2/3O₂ cathode also exhibited notable durability with 97.2% capacity retention after 300 cycles. This outstanding performance is attributed to the distinctive three-dimensional network structure of the very-fine Fe₂O₃ nanoparticles uniformly embedded in the interconnected porous N-doped carbon nanofibers that effectively facilitated electronic/ionic transport and prevented active materials pulverization/aggregation caused by volume change upon prolonged cycling. The simple and scalable preparation route, as well as the excellent electrochemical performance, endows the Fe₂O₃@C nanofibers with great prospects as high-rate and long-life Na-storage anode materials.

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Graphene and cobalt phosphide nanowire composite as an anode material for high performance lithium-ion batteries

The synthesis of a composite of cobalt phosphide nanowires and reduced graphene oxide (denoted CoP/RGO) via a facile hydrothermal method combined with a subsequent annealing step is reported. The resulting composite presents large specific surface area and enhanced conductivity, which can effectively facilitate charge transport and accommodates variations in volume during the lithiation/de-lithiation processes. As a result, the CoP/RGO nanocomposite manifests a high reversible specific capacity of 960 mA·h·g^–1 over 200 cycles at a current density of 0.2 A·g^–1 (297 mA·h·g^–1 over 10,000 cycles at a current density of 20 A·g^–1) and excellent rate capability (424 mA·h·g^–1 at a current density of 10 A·g^–1).

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MOF-derived carbon coating on self-supported ZnCo<Subscript>2</Subscript>O<Subscript>4</Subscript>–ZnO nanorod arrays as high-performance anode for lithium-ion batteries

The C–ZnCo₂O₄–ZnO nanorod arrays (NRAs), which consist of MOF-derived carbon coating on ZnCo₂O₄–ZnO NRAs, are rational designed and synthesized via a facile template-based solution route on Ti foil and used as high-performance anode for lithium-ion batteries (LIBs). The uniform coated MOF-derived carbon layers on the ZnCo₂O₄–ZnO nanorods surface can serve as a conductive substrate as well as buffer layer to restrain volume expansion during charge–discharge process. When tested as anodes for LIBs, the C–ZnCo₂O₄–ZnO NRAs show high reversible capacity of 1318 mA h g^?1 at 0.2 A g^?1 after 150 charge–discharge cycles. Furthermore, C–ZnCo₂O₄–ZnO NRAs also exhibit brilliant rate performance of 886.2, 812.8, 732.2 and 580.6 mA h g^?1 at 0.5, 1, 2 and 5 A g^?1, respectively. The outstanding lithium storage performance of C–ZnCo₂O₄–ZnO NRAs could be ascribed to the stimulated kinetics of ion diffusion and electron transport originated from the shortened lithium-ion diffusion pathway and improved electronic conductivity benefit from uniformly coating MOF-derived carbon.     

Construction of point-line-plane (0-1-2 dimensional) Fe<Subscript>2</Subscript>O<Subscript>3</Subscript>-SnO<Subscript>2</Subscript>/graphene hybrids as the anodes with excellent lithium storage capability

The assembly of hybrid nanomaterials has opened up a new direction for the construction of high-performance anodes for lithium-ion batteries (LIBs). In this work, we present a straightforward, eco-friendly, one-step hydrothermal protocol for the synthesis of a new type of Fe₂O₃-SnO₂/graphene hybrid, in which zero-dimensional (0D) SnO₂ nanoparticles with an average diameter of 8 nm and one-dimensional (1D) Fe₂O₃ nanorods with a length of ~150 nm are homogeneously attached onto two-dimensional (2D) reduced graphene oxide nanosheets, generating a unique point-line-plane (0D-1D-2D) architecture. The achieved Fe₂O₃-SnO₂/graphene exhibits a well-defined morphology, a uniform size, and good monodispersity. As anode materials for LIBs, the hybrids exhibit a remarkable reversible capacity of 1,530 mA·g^?1 at a current density of 100 mA·g^?1 after 200 cycles, as well as a high rate capability of 615 mAh·g^?1 at 2,000 mA·g^?1. Detailed characterizations reveal that the superior lithium-storage capacity and good cycle stability of the hybrids arise from their peculiar hybrid nanostructure and conductive graphene matrix, as well as the synergistic interaction among the components.

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Composite of sulfur impregnated in porous hollow carbon spheres as the cathode of Li-S batteries with high performance

Carbon-sulfur composites as the cathode of rechargeable Li-S batteries have shown outstanding electrochemical performance for high power devices. Here, we report the promising electrochemical charge-discharge properties of a carbon-sulfur composite, in which sulfur is impregnated in porous hollow carbon spheres (PHCSs) via a melt-diffusion method. Instrumental analysis shows that the PHCSs, which were prepared by a facile template strategy, are characterized by high specific surface area (1520 m²·g^?1), large pore volume (2.61 cm³·g^?1), broad pore size distribution from micropores to mesopores, and high electronic conductivity (2.22 S·cm^?1). The carbon-sulfur composite with a sulfur content of 50.2 wt.% displays an initial discharge capacity of 1450 mA·h·g^?1 (which is 86.6% of the theoretical specific capacity) and a reversible discharge capacity of 1357 mA·h·g^?1 after 50 cycles at 0.05 C charge-discharge rate. At a higher rate of 0.5C, the capacity stabilized at around 800 mA·h·g^?1 after 30 cycles. The results illustrate that the porous carbon-sulfur composites with hierarchically porous structure have potential application as the cathode of Li-S batteries because of their effective improvement of the electronic conductivity, the repression of the volume expansion, and the reduction of the shuttling loss.      

Rational design and synthesis of hierarchically structured SnO<Subscript>2</Subscript> microspheres assembled from hollow porous nanoplates as superior anode materials for lithium-ion batteries

Herein, hierarchically structured SnO₂ microspheres are designed and synthesized as an efficient anode material for lithium-ion batteries using hollow SnO₂ nanoplates. Three-dimensionally ordered macroporous (3-DOM) SnO _x -C microspheres synthesized by spray pyrolysis are transformed into hierarchically structured SnO₂ microspheres by a two-step post-treatment process. Sulfidation produces hierarchically structured SnS-SnS₂-C microspheres comprising tin sulfide nanoplate and carbon building blocks. A subsequent oxidation process produces SnO₂ microspheres from hollow SnO₂ nanoplate building blocks, which are formed by Kirkendall diffusion. The discharge capacity of the hierarchically structured SnO₂ microspheres at a current density of 5 A·g^?1 for the 600^th cycle is 404 mA·h·g^?1. The hierarchically structured SnO₂ microspheres have reversible discharge capacities of 609 and 158 mA·h·g^?1 at current densities of 0.5 and 30 A·g^?1, respectively. The ultrafine nanosheets contain empty voids that allow excellent lithium-ion storage performance, even at high current densities.

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Ni-doped ZnCo<Subscript>2</Subscript>O<Subscript>4</Subscript> atomic layers to boost the selectivity in solar-driven reduction of CO<Subscript>2</Subscript>

Regulating the selectivity of CO₂ photoreduction is particularly challenging. Herein, we propose ideal models of atomic layers with/without element doping to investigate the effect of doping engineering to tune the selectivity of CO₂ photoreduction. Prototypical ZnCo₂O₄ atomic layers with/without Ni-doping were first synthesized. Density functional theory calculations reveal that introducing Ni atoms creates several new energy levels and increases the density-of-states at the conduction band minimum. Synchrotron radiation photoemission spectroscopy demonstrates that the band structures are suitable for CO₂ photoreduction, while the surface photovoltage spectra demonstrate that Ni doping increases the carrier separation efficiency. In situ diffuse reflectance Fourier transform infrared spectra disclose that the CO₂^·? radical is the main intermediate, while temperature-programed desorption curves reveal that the ZnCo₂O₄ atomic layers with/without Ni doping favor the respective CO and CH₄ desorption. The Ni-doped ZnCo₂O₄ atomic layers exhibit a 3.5-time higher CO selectivity than the ZnCo₂O₄ atomic layers. This work establishes a clear correlation between elemental doping and selectivity regulation for CO₂ photoreduction, opening new possibilities for tailoring solar-driven photocatalytic behaviors.

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Encapsulation of selenium sulfide in double-layered hollow carbon spheres as advanced electrode material for lithium storage

Selenium sulfide/double-layered hollow carbon sphere (SeS₂/DLHC) composites have been designed as high-performance cathode materials for novel Li–SeS₂ batteries. In the constructed composite, SeS₂ is predominantly encapsulated in the interlayer space of DLHCs with a high loading of 75% (weight percentage) and serves as the active component for lithium storage. The presence of Se in the composite and the carbon framework not only alleviate the shuttling of polysulfide, but also improve the conductivity of electrodes. Migration of active materials from the interlayer void to the hollow cavity of DLHCs after cycling, which further mitigates the loss of active materials and the shuttle effect, is observed. As a result, the SeS₂/DLHC composite delivers a high specific capacity (930 mA·h·g^?1 at 0.2 C) and outstanding rate capability (400 mA·h·g^?1 at 6 C), which is much better than those of SeS₂/single-layered hollow carbon sphere, Se/DLHC, and S/DLHC composites. Notably, the SeS₂/DLHC composite shows an ultralong cycle life with 89% capacity retention over 900 cycles at 1 C, or only 0.012% capacity decay per cycle. Our study reveals that both SeS₂ and the double-layered structures are responsible for the excellent electrochemical performance.

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Multi-dimensionally ordered,multi-functionally integrated r-GO@TiO<Subscript>2</Subscript>(B)@Mn<Subscript>3</Subscript>O<Subscript>4</Subscript> yolk–membrane–shell superstructures for ultrafast lithium storage

TiO₂(B) is an attractive new anode candidate for lithium-ion batteries (LIBs) due to its unique and highly desirable properties, including high structural integrity, long cycle life, and low cost. However, despite these merits, its inherent slow lithium and electron transport kinetics hinder its practical application to LIBs. Here, we propose a novel, simple route towards multi-dimensionally ordered, multi-functionally integrated reduced graphene oxide (r-GO)@TiO₂(B)@Mn₃O₄ yolk–membrane–shell superstructures in which r-GO nanosheets, TiO₂(B) nanosheets, and Mn₃O₄ nanoparticles are hierarchically organized to achieve remarkable synergistic interactions. This hybridization design is fundamentally bilateral in nature, aiming to overcome the conductivity and capacity deficiencies of TiO₂(B) simultaneously. The resulting r-GO@TiO₂(B)@Mn₃O₄ yolk–membrane–shell superstructures have great potential as advanced anode materials for ultrafast lithium storage, delivering a strikingly high reversible capacity of 662 mA·h·g^?1 at 500 mA·g^?1 after 500 charge–discharge cycles.

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Spin-coated silicon nanoparticle/graphene electrode as a binder-free anode for high-performance lithium-ion batteries

Si has been considered as a promising anode material but its practical application has been severely hindered due to poor cyclability caused by the large volume change during charge/discharge. A new and effective protocol has been developed to construct Si nanoparticle/graphene electrodes with a favorable structure to alleviate this problem. Starting from a stable suspension of Si nanoparticles and graphene oxide in ethanol, spin-coating can be used as a facile method to cast a spin-coated Si nanoparticle/graphene (SC-Si/G) film, in which graphene can act as both an efficient electronic conductor and effective binder with no need for other binders such as polyvinylidenefluoride (PVDF) or polytetrafluoroethylene (PTFE). The prepared SC-Si/G electrode can achieve a high-performance as an anode for lithium-ion batteries benefiting from the following advantages: i) the graphene enhances the electronic conductivity of Si nanoparticles and the void spaces between Si nanoparticles facilitate the lithium ion diffusion, ii) the flexible graphene and the void spaces can effectively cushion the volume expansion of Si nanoparticles. As a result, the binder-free electrode shows a high capacity of 1611 mA·h·g^?1 at 1 A·g^?1 after 200 cycles, a superior rate capability of 648 mA·h·g^?1 at 10 A·g^?1, and an excellent cycle life of 200 cycles with 74% capacity retention.      

A new sodium iron phosphate as a stable high-rate cathode material for sodium ion batteries

Low-cost room-temperature sodium-ion batteries (SIBs) are expected to promote the development of stationary energy storage applications. However, due to the large size of Na⁺, most Na⁺ host structures resembling their Li+ counterparts show sluggish ion mobility and destructive volume changes during Na ion (de)intercalation, resulting in unsatisfactory rate and cycling performances. Herein, we report a new type of sodium iron phosphate (Na_0.71Fe_1.07PO₄), which exhibits an extremely small volume change (~ 1%) during desodiation. When applied as a cathode material for SIBs, this new phosphate delivers a capacity of 78 mA·h·g^?1 even at a high rate of 50 C and maintains its capacity over 5,000 cycles at 20 C. In situ synchrotron characterization disclosed a highly reversible solid-solution mechanism during charging/discharging. The findings are believed to contribute to the development of high-performance batteries based on Earth-abundant elements.

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Facile synthesis and electrochemical sodium storage of CoS<Subscript>2</Subscript> micro/nano-structures

We report the synthesis and electrochemical sodium storage of cobalt disulfide (CoS₂) with various micro/nano-structures. CoS₂ with microscale sizes are either assembled by nanoparticles (P-CoS₂) via a facile solvothermal route or nanooctahedrons constructed solid (O-CoS₂) and hollow microstructures (H-CoS₂) fabricated by hydrothermal methods. Among three morphologies, H-CoS₂ exhibits the largest discharge capacities and best rate performance as anode of sodium-ion batteries (SIBs). Furthermore, H-CoS₂ delivers a capacity of 690 mA·h·g^?1 at 1 A·g^?1 after 100 cycles in a potential range of 0.1–3.0 V, and ～240 mA·h·g^?1 over 800 cycles in the potential window of 1.0–3.0 V. This cycling difference mainly lies in the two discharge plateaus observed in 0.1–3.0 V and one discharge plateau in 1.0–3.0 V. To interpret the reactions, X-ray diffraction (XRD) and transmission electron microscopy (TEM) are applied. The results show that at the first plateau around 1.4 V, the insertion reaction (CoS₂ + xNa⁺ + xe^? → Na _x CoS₂) occurs; while at the second plateau around 0.6 V, the conversion reaction (Na _x CoS₂ + (4 ? x) Na⁺ + (4 ? x)e^? → Co + 2Na₂S) takes place. This provides insights for electrochemical sodium storage of CoS₂ as the anode of SIBs.

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Yolk–shell-structured (Fe0.5Ni0.5)9S8 solid-solution powders: Synthesis and application as anode materials for Na-ion batteries

Multicomponent metal sulfide materials with a yolk–shell structure and a single phase were studied for the first time as anode materials for sodium-ion batteries. Yolk–shell-structured Fe–Ni–O powders with a molar ratio of iron and nickel components of 1/1 were prepared via one-pot spray pyrolysis. The prepared Fe–Ni–O powders were transformed into yolk–shell-structured (Fe_0.5Ni_0.5)₉S₈ solid-solution powders via a sulfidation process. The initial discharge and charge capacities of the (Fe_0.5Ni_0.5)₉S₈ powders at a current density of 1 A·g⁻¹ were 601 and 504 mA·h·g⁻¹, respectively. The discharge capacities of the (Fe_0.5Ni_0.5)₉S₈ powders for the 2^nd and 100^th cycle were 530 and 527 mA·h·g⁻¹, respectively, and their corresponding capacity retention measured from the 2^nd cycle was 99%. The (Fe_0.5Ni_0.5)₉S₈ powders had high initial discharge and charge capacities at a low current density of 0.1 A·g⁻¹, and the reversible discharge capacity decreased slightly from 568 to 465 mA·h·g⁻¹ as the current density increased from 0.1 to 5.0 A·g⁻¹. The synergetic effect of the novel yolk–shell structure and the multicomponent sulfide composition of the (Fe_0.5Ni_0.5)₉S₈ powders resulted in excellent sodium-ion storage performance.

     

Sandwich-structured nanocomposites of N-doped graphene and nearly monodisperse Fe<Subscript>3</Subscript>O<Subscript>4</Subscript> nanoparticles as high-performance Li-ion battery anodes

Iron oxides have attracted considerable interest as abundant materials for high-capacity Li-ion battery anodes. However, their fast capacity fading owing to poorly controlled reversibility of the conversion reactions greatly hinders their application. Here, a sandwich-structured nanocomposite of N-doped graphene and nearly monodisperse Fe₃O₄ nanoparticles were developed as high-performance Li-ion battery anode. N-doped graphene serves as a conducting framework for the self-assembled structure and controls Fe₃O₄ nucleation through the interaction of N dopants, surfactant molecules, and iron precursors. Fe₃O₄ nanoparticles were well dispersed with a uniform diameter of ~15 nm. The unique sandwich structure enables good electron conductivity and Li-ion accessibility and accommodates a large volume change. Hence, it delivers good cycling reversibility and rate performance with a capacity of ~1,227 mA·h·g^–1 and 96.8% capacity retention over 1,000 cycles at a current density of 3 A·g^–1. Our work provides an ideal structure design for conversion anodes or other electrode materials requiring a large volume change.

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Synthesis of well-defined Fe<Subscript>3</Subscript>O<Subscript>4</Subscript> nanorods/N-doped graphene for lithium-ion batteries

The geometric size and distribution of magnetic nanoparticles are critical to the morphology of graphene (GN) nanocomposites, and thus they can affect the capacity and cycling performance when these composites are used as anode materials in lithium-ion batteries (LiBs). In this work, Fe₃O₄ nanorods were deposited onto fully extended nitrogen-doped GN sheets from a binary precursor in two steps, a hydrothermal process and an annealing process. This route effectively tuned the Fe₃O₄ nanorod size distribution and prevented their aggregation. The transformation of the binary precursor was characterized by X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), and transmission electron microscopy (TEM). XPS analysis indicated the presence of N-doped GN sheets, and that the magnetic nanocrystals were anchored and uniformly distributed on the surface of the flattened N-doped GN sheets. As a high performance anode material, the structure was beneficial for electron transport and exchange, resulting in a large reversible capacity of 929 mA·h·g^–1, high-rate capability, improved cycling stability, and higher electrical conductivity. Not only does the result provide a strategy for extending GN composites for use as LiB anode materials, but it also offers a route for the preparation of other oxide nanorods from binary precursors.

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Low-cost disordered carbons for Li/S batteries: A high-performance carbon with dual porosity derived from cherry pits

A micro- and mesoporous carbon obtained from cherry pit waste and activated with H₃PO₄ acid has been studied as the sulfur host for Li/S batteries. The carbon has a high specific surface area of 1,662 m²·g^–1 (SBET) and micropore and mesopore volumes of 0.57 and 0.40 cm³·g^–1, respectively. The S/C composite, with a sulfur content of 57% deposited by the disproportionate reaction of a S₂O₃ ^2? solution in an acid medium without an additional heating step above the S melting point, delivers an initial specific capacity of 1,148 mAh·g^–1 at a current of C/16. It also has a high capacity retention of 915 mAh·g^–1 after 100 cycles and a Coulombic efficiency close to 100%. The good performance of the composite was also observed under higher current rates and long-term cycling tests. The capacities delivered by the cell after 200 cycles were 707 and 410 mAh·g^–1 at C/2 and 1C (1C = 1,675 mA·g^–1), respectively, maintaining the high Coulombic efficiency. The overall electrochemical response of this carbon as the sulfur matrix is among the best reported so far among the other biomass-derived carbons, probably because of the micro- and mesopore system formed upon activation.

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