Facilitating sulfur species capture and bi-directional redox in Li-S batteries with single-atomic Co-O_(2)N_(2) coordination structure

Lithium-sulfur(Li-S)batteries suffer from the shuttle effect of soluble lithium polysulfides(LiPSs)and slow redox kinetics,significantly limiting their practical application.Although single-atom catalysts(SACs)offer a promising strategy to address these challenges,designing materials with optimal adsorption force and high catalytic activity remains a grand challenge.Here,we present a cobalt(Co)-based SAC with unique Co-O_(2)N_(2) coordination structures for Li-S batteries.Both experimental and theoretical studies demonstrate that O,N-coordinated Co single atoms anchored on a porous carbon framework(Co/NOC)effectively capture LiPSs and dramatically catalyze bidirectional polysulfide conversion.The expanded carbon layer spacing facilitates lithium ions diffusion and maximizes the exposure of active sites.As a result,Li-S batteries incorporating Co/NOC as separators exhibit outstanding rate performance(906.6m Ah g^(-1)at 3 C)and exceptional cycling stability,even at-10℃.Furthermore,with a high sulfur loading of 12.0 mg cm^(-2),the areal specific capacity reaches up to 12.36 mAh cm^(-2).This work provides some useful insights for the design of high-performance SACs for Li-S batteries.

Vanadium oxide nanospheres encapsulated in N-doped carbon nanofibers with morphology and defect dual-engineering toward advanced aqueous zinc-ion batteries

Vanadium-based electrodes are regarded as attractive cathode materials in aqueous zinc ion batteries(ZIBs)caused by their high capacity and unique layered structure.However,it is extremely challenging to acquire high electrochemical performance owing to the limited electronic conductivity,sluggish ion kinetics,and severe volume expansion during the insertion/extraction process of Zn^(2+).Herein,a series of V_(2)O_(3)nanospheres embedded N-doped carbon nanofiber structures with various V_(2)O_(3)spherical morphologies(solid,core-shell,hollow)have been designed for the first time by an electrospinning technique followed thermal treatments.The N-doped carbon nanofibers not only improve the electrical conductivity and the structural stability,but also provides encapsulating shells to prevent the vanadium dissolution and aggregation of V_(2)O_(3)particles.Furthermore,the varied morphological structures of V_(2)O_(3)with abundant oxygen vacancies can alleviate the volume change and increase the Zn^(2+)pathway.Besides,the phase transition between V_(2)O_(3)and Zn_XV_(2)O_(5-m)·n H_(2)O in the cycling was also certified.As a result,the as-obtained composite delivers excellent long-term cycle stability and enhanced rate performance for coin cells,which is also confirmed through density functional theory(DFT)calculations.Even assembled into flexible ZIBs,the sample still exhibits superior electrochemical performance,which may afford new design concept for flexible cathode materials of ZIBs.

Synthesis of well-defined Fe3O4 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, Fe304 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.

Porous-hollow nanorods constructed from alternate intercalation of carbon and MoS2 monolayers for lithium and sodium storage

Weak ion diffusion and electron transport due to limited interlayer spacing and poor electrical conductivity have been identified as critical roadbacks for fast and abundant energy storage of both MoS2-based lithium ion batteries (LIBs) and sodium ion batteries (SIBs). In this work, MoS2 porous-hollow nanorods (MoS2/m-C800) have been designed and synthesized via an annealing-followed chemistry-intercalated strategy to solve the two issues. They are uniformly assembled from ultrathin MoS2 nanosheets, deviated to the rod-axis direction, with expanded interlayer spacing due to alternate intercalation of N-doped carbon monolayers between the adjacent MoS2 monolayers. Electrochemical studies of the MoS2/m-C800 sample, as an anode of LIBs, demonstrate that the superstructure can deliver a reversible discharge capacity of 1,170 mAh·g^-1 after 100 cycles at 0.2 A·g^-1 and maintain a reversible capacity of 951 mAh·g^-1 at 1.25 A·g^-1 after 350 cycles. While for SIBs, the superstructure also delivers a reversible discharge capacity of 350 mAh·g^-1 at 0.5 A-g-1 after 500 cycles and exhibits superior rate capacity of 238 mAh·g^-1 at 15 A·g^-1 .The excellent electrochemical performance is closely related with the hierarchical superstructures, including expanded interlayer spacing, alternate intercalation of carbon monolayers and mesoporous feature, which effectively reduce ion diffusion barrier, shorten ion diffusion paths and improve electrical conductivity.

MoS2-intercalated carbon hetero-layers bonded on graphene as electrode materials for enhanced sodium/potassium ion storage

MoS2 is considered as an ideal electrode material in the field of energy storage due to high theoretical specific capacity and unique layered structure.However,limited interlayer distance and poor intrinsic electrical conductivity restrict its potential realworld application.Herein,an alternately intercalated structure of MoS2 monolayer and N-doped porous carbon(NC)layer is grown on reduced graphene oxide(rGO)via a chemical intercalated strategy.The expanded interlayer distance of MoS2(0.96 nm),enlarged by the intercalation of N-doped porous carbon layers,can enhance ion diffusion mobility,provide additional reactive sites for ion storage and maintain the stability of electrode structure.In addition,the hierarchical structures between rGO substrate and intercalated N-doped carbon layers construct a three-dimensional(3D)conductive network,which can significantly improve the electrical conductivity and the structural stability.As a result,the rGO-supported MoS2/NC electrode exhibits an ultrahigh reversible capacity and remarkable long cycling stability for sodium-ion batteries(SIBs)and potassium-ion(PIBs).Meanwhile,the as-obtained MoS2/NC@rGO electrode also delivers a superior cycle performance of 250 mAh·g−1 after 160 cycles at 0.5 A·g−1 when employed as an anode for sodium-ion full cells.

Assembly of flower-like VS_(2)/N-doped porous carbon with expanded(001)plane on rGO for superior Na-ion and K-ion storage

VS2 with natural layered structure and metallic conductivity is a prospective candidate for sodium-ion batteries(SIBs)and potassium-ion batteries(PIBs).However,due to large radius of Na+and K+,the limited interlayer spacing(0.57 nm)of VS2 generally determines high ion diffusion barrier and large volume variation,resulting in unsatisfactory electrochemical performance of SIBs and PIBs.In this work,flower-like VS_(2)/N-doped carbon(VS_(2)/N-C)with expanded(001)plane is grown on reduced graphene oxide(rGO)via a solvothermal and subsequently carbonization strategy.In the VS_(2)/N-C@rGO nanohybrids,the ultrathin VS2"petals"are alternately intercalated by the N-doped porous carbon monolayers to achieve an expanded interlayer spacing(1.02 nm),which can effectively reduce ions diffusion barrier,expose abundant active sites for Na+/K+intercalation,and tolerate large volume variation.The N-C and rGO carbonous materials can significantly promote the electrical conductivity and structural stability.Benefited from the synergistic effect,the VS2/N-C@rGO electrode exhibits large reversible capacity(Na+:407 mAh·g^(-1) at 1 A·g^(-1);K^(+):334 mAh·g^(-1) at 0.2 A·g^(-1)),high rate capacity(Na+:273 mAh·g^(-1) at 8 A·g^(-1);K+:186 mAh·g^(-1) at 5 A·g^(-1)),and remarkable cycling stability(Na+:316 mAh·g^(-1) at 2 A·g^(-1) after 1,400 cycles;K^(+):216 mAh·g^(-1) at 1 A·g^(-1) after 500 cycles).