Synthesis and electrochemical performance of sulfur–carbon composite cathode for lithium–sulfur batteries

In this paper, porous carbon was synthesized by an activation method, with phenolic resin as carbon source and nanometer calcium carbonate as activating agent. Sulfur–porous carbon composite material was prepared by thermally treating a mixture of sublimed sulfur and porous carbon. Morphology and electrochemical performance of the carbon and sulfur–carbon composite cathode were investigated by X-ray diffraction (XRD), scanning electron microscopy (SEM), cyclic voltammetry (CV), electrochemical impedance spectra (EIS), and galvanostatic charge–discharge test. The composite containing 39 wt.% sulfur obtained an initial discharge capacity of about 1,130 mA?h g^?1 under the current density of 80 mA?g^?1 and presented a long electrochemical stability up to 100 cycles.     

Nano-wire networks of sulfur–polypyrrole composite cathode materials for rechargeable lithium batteries

Polypyrrole (PPy) nanowire was synthesized through a surfactant mediated approach. The sulfur–polypyrrole (S–PPy) composite materials were prepared by heating the mixture of element sulfur and polypyrrole nanowire. The materials were characterized by FTIR, SEM. PPy with special morphology serves as conductive additive, distribution agent and absorbing agents, which effectively enhanced the electrochemical performance of sulfur. The initial discharge capacity of the active materials was 1222 mA h g⁻¹ the remaining capacity is 570 mA h g⁻¹ after 20th cycles.     

Synthesis and electrochemical performance of TiO2–sulfur composite cathode materials for lithium–sulfur batteries

Titania–sulfur (TiO₂–S) composite cathode materials were synthesized for lithium–sulfur batteries. The composites were characterized and examined by X-ray diffraction, nitrogen adsorption/desorption measurements, scanning electron microscopy, and electrochemical methods, such as cyclic voltammetry, electrochemical impedance spectroscopy, and galvanostatic charge–discharge tests. It is found that the mesoporous TiO₂ and sulfur particles are uniformly distributed in the composite after a melt-diffusion process. When evaluating the electrochemical properties of as-prepared TiO₂–S composite as cathode materials in lithium–sulfur batteries, it exhibits much improved cyclical stability and high rate performance. The results showed that an initial discharge specific capacity of 1,460 mAh/g at 0.2 C and capacity retention ratio of 46.6 % over 100 cycles of composite cathode, which are higher than that of pristine sulfur. The improvements of electrochemical performances were due to the good dispersion of sulfur in the pores of TiO₂ particles and the excellent adsorbing effect on polysulfides of TiO₂.     

Synthesis and application of single-atom catalysts in sulfur cathode for high-performance lithium–sulfur batteries

Lithium–sulfur(Li-S) batteries are regarded as one of the most promising energy storage devices because of their low cost, high energy density, and environmental friendliness. However, Li-S batteries suffer from sluggish reaction kinetics and serious “shuttle effect” of lithium polysulfides(LiPSs), which causes rapid decay of battery capacity and prevent their practical application. To address these problems, introducing single-atom catalysts(SACs) is an effective method to improve the electroch...     

Three-dimensionally interconnected Co9S8/MWCNTs composite cathode host for lithium–sulfur batteries

Several challenging issues,such as the poor conductivity of sulfur,shuttle effects,large volume change of cathode,and the dendritic lithium in anode,have led to the low utilization of sulfur and hampered the commercialization of lithium–sulfur batteries.In this study,a novel three-dimensionally interconnected network structure comprising Co9 S8 and multiwalled carbon nanotubes(MWCNTs)was synthesized by a solvothermal route and used as the sulfur host.The assembled batteries delivered a specific capacity of1154 m Ah g-1 at 0.1 C,and the retention was 64%after 400 cycles at 0.5 C.The polar and catalytic Co9 S8 nanoparticles have a strong adsorbent effect for polysulfide,which can effectively reduce the shuttling effect.Meanwhile,the three-dimensionally interconnected CNT networks improve the overall conductivity and increase the contact with the electrolyte,thus enhancing the transport of electrons and Li ions.Polysulfide adsorption is greatly increased with the synergistic effect of polar Co9 S8 and MWCNTs in the three-dimensionally interconnected composites,which contributes to their promising performance for the lithium–sulfur batteries.     

Carbon fiber-incorporated sulfur/carbon ternary cathode for lithium–sulfur batteries with enhanced performance

Journal of Solid State Electrochemistry - Smart construction of advanced sulfur cathodes is indispensable for the development of high performance lithium–sulfur (Li–S) batteries. Hence,...     

An odyssey of lithium metal anode in liquid lithium–sulfur batteries

Lithium–sulfur (Li–S) batteries exhibit outstanding energy density and material sustainability. Enormous effects have been devoted to the sulfur cathode to address redox kinetics and polysulfide intermediates shuttle. Recent attentions are gradually turning to the protection of the lithium metal anodes, since electrochemical performances of Li–S batteries are closely linked to the working efficiency of the anode side, especially in pouch cells that adopt stringent test protocols. This Perspective article summarizes critical issues encountered in the lithium metal anode, and outlines possible solutions to achieve efficient working lithium anode in Li–S batteries. The lithium metal anode in Li–S batteries shares the common failure mechanisms of volume fluctuation, nonuniform lithium flux, electrolyte corrosion and lithium pulverization occurring in lithium metal batteries with oxide cathodes, and also experiences unique polysulfide corrosion and massive lithium accumulation. These issues can be partially addressed by developing three-dimensional scaffold, exerting quasi-solid reaction, tailoring native solid electrolyte interphase (SEI) and designing artificial SEI. The practical evaluation of Li–S batteries highlights the importance of pouch cell platform, which is distinguished from coin-type cells in terms of lean electrolyte-to-sulfur ratio, thin lithium foil, as well as sizable total capacity and current that are loaded on pouch cells. This Perspective underlines the development of practically efficient working lithium metal anode in Li–S batteries.     

A novel modified sulfur cathode to facilitate the adsorption and conversion of polysulfides in lithium–sulfur batteries

Journal of Solid State Electrochemistry - Physical confinement through particular nanostructures is inadequate to avoid the shuttle effect in the lithium–sulfur batteries. Electrocatalysts...     

Hierarchically porous nitrogen-doped carbon as cathode for lithium–sulfur batteries

Porous nitrogen-doped carbon is an especially promising material energy storage due to its excellent conductivity, stable physicochemical properties, easy processability, controllable porosity and low price.Herein, we reported a novel well-designed hierarchically porous nitrogen-doped carbon(HPNC) via a combination of salt template(ZnCl_2) and hard template(SiO_2) as sulfur host for lithium–sulfur batteries. The low-melting ZnCl_2 is boiled off and leaves behind micropores and small size mesopores during pyrolysis process, while the silica spheres are removed by acid leaching to generate interconnected 3D network of macropores. The HPNC-S electrode exhibits an initial specific capacity of 1355 mAh g~(–1) at 0.1 C(1 C = 1675 m Ah g~(–1)), a high-rate capability of 623 m Ah g~(–1) at 2 C, and a small decay of 0.13% per cycle over 300 cycles at 0.2 C. This excellent rate capability and remarkable long-term cyclability of the HPNC-S electrode are attributed to its hierarchical porous structures for confining the soluble lithium polysulfide as well as the nitrogen doping for high absorbability of lithium polysulfide.     

Grafting polymeric sulfur onto carbon nanotubes as highly-active cathode for lithium–sulfur batteries

Lithium–sulfur(Li–S)batteries are being explored as promising advanced energy storage systems due to their ultra-high energy density.However,fast capacity fading and low coulombic efficiency,resulting from the dissolution of polysulfides,remain a serious challenge.Compared to weak physical adsorptions or barriers,chemical confinement based on strong chemical interaction is a more effective approach to address the shuttle issue.Herein,we devise a novel polymeric sulfur/carbon nanotube composite for Li–S battery,for which 2,5-dithiobiurea is chosen as the stabilizer of long-chain sulfur.This offers chemical bonds which bridge the polymeric sulfur and carbon nanotubes.The obtained composite can deliver an ultra-high reversible capacity of 1076.2 m Ah g~(-1)(based on the entire composite)at the rate of 0.1 C with an exceptional initial Coulombic efficiency of 96.2%,as well as remarkable cycle performance.This performance is mainly attributed to the reaction reversibility of the obtained polymeric sulfur-based composite during the discharge/charge process.This was confirmed by density functional theory calculations for the first time.     

Core@shell sulfur@polypyrrole nanoparticles sandwiched in graphene sheets as cathode for lithium–sulfur batteries

A nano sulfur-based composite cathode material featured by uniform core@shell-structured sulfur@polypyrrole nanoparticles sandwiched in three-dimensional graphene sheets conductive network(S@PPy/GS) is fabricated via a facile solution-based method. The S@PPy nanoparticles are synthesized by in situ chemical oxidative polymerization of pyrrole on the surface of sulfur particles,and then graphene sheets are covered outside the S@PPy nanoparticles,forming a three-dimensional conductive network. When evaluating the electrochemical performance of S@PPy/GS in a lithium–sulfur battery,it delivers large discharge capacity,excellent cycle stability,and good rate capability. The initial discharge capacity is up to 1040 m Ah/g at 0.1 C,the capacity can remain 537.8 m Ah/g at 0.2 C after 200 cycles,even at a higher rate of 1 C,the specific capacity still reaches 566.5 m Ah/g. The good electrochemical performance is attributed to the unique structure of S@PPy/GS,which can not only provide an excellent transport of lithium and electron ions within the electrodes,but also retard the shuttle effect of soluble lithium polysulfides effectively,thus plays a positive role in building better lithium-sulfur batteries.     

Enhanced performance of lithium polymer batteries using a V2O5–PEG composite cathode

A new concept is proposed to realize solid-state high-performance lithium polymer batteries in which two different polymers are used as ionically conductive matrices in the cathode and in the separator. A solid, low molecular weight poly(ethylene glycol) was used in the cathode while a blend with a higher molecular weight poly(ethylene oxide) (PEO) was used in the separator. The enhanced transport properties in the cathodic compartment allow us to discharge the battery (190 mAh g⁻¹) at a moderate temperature (65°C) in a reasonable time (about 3.3 h). Batteries cycled at 100°C showed enhanced performance with respect to PEO-based batteries. At a power density of about 416 W kg⁻¹, energy density as high as 460 Wh kg⁻¹, based on the weight of the active material, was achieved in about 1 h of discharge. The work was developed within the ALPE (Advanced Lithium Polymer Electric Vehicle Battery) project, an Italian integrated project devoted to the realization of lithium polymer batteries for electric vehicle applications, in collaboration with the Osaka National Research Institute.     

Preparation of yolk-shell sulfur/carbon nanocomposite via an organic solvent route for lithium–sulfur batteries

A yolk-shell sulfur/carbon (S/C) composite for the cathode of lithium–sulfur batteries was successfully prepared by an accessible method with tetrahydrofuran as solvent. The as-prepared composites are characterized by thermal gravimetric, X-ray diffraction, field emission scanning electron microscopy, transmission electron microscopy, and nitrogen adsorption and desorption. In this composite, sulfur particle is encapsulated in the carbon shell even entering into the micropores of carbon Bp2000. The electrochemical performance of the S/C composites is evaluated. The results indicate that the S/C composite with 50 wt% sulfur content shows good reversibility, excellent rate capability, and slow degradation. It delivers an initial capacity of 784.4 mAh g^?1 (based on sulfur weight) and preserves at 598.3 mAh g^?1 after 195 cycles at 1C. It achieves a high-capacity retention of 76.27 % from the 5th to 200th cycle, and as high as 91.19 % during the latter 150 cycles. The improvement is mainly attributed to the favorable structure of the S/C composite, in which the carbon cannot only facilitate transport of electrons and Li⁺ ions but also trap polysulfides and retard the shuttle effect during charge/discharge process.     

Electrocatalysis of polysulfide conversion via sulfur–cobalt CoS2 on a carbon nanotube surface as a cathode for high-performance lithium–sulfur batteries

Journal of Solid State Electrochemistry - Lithium–sulfur batteries received intense attention because of their high-energy density and inexpensive active material. However, the poor...     

Insight into demand-driven preparation of single-atomic mediators for lithium–sulfur batteries

Lithium-sulfur(Li-S) batteries have attracted considerable attention as one of the most appealing energy storage systems.Strenuous efforts have been devoted to tackling the tremendous challenges,mainly pertaining to the severe shuttle effect,sluggish redox kinetics and lithium dendritic growth.Single-atomic mediators as promising candidates exhibit impressive performance in addressing these intractable issues.Related research often utilizes a trial-and-error approach,proposing solutions to fabri...     

A comparison of sulfur loading method on the electrochemical performance of porous carbon/sulfur cathode material for lithium–sulfur battery

To get a high sulfur loaded porous carbon/sulfur cathode material with an excellent performance, we investigated four different sulfur loading treatments. The samples were analyzed by the Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD) patterns, thermal gravimetric analysis (TGA), and scanning electron microscopy (SEM). We proved that it is more effective to introduce the sulfur into the pores of porous carbon at 300 °C than at 155 °C. Especially, the porous carbon/sulfur composite heated in a sealed reactor at 300 °C for 8 h presents a fine sulfur load with sulfur content of 78 wt.% and exhibits an excellent electrochemical performance. The discharge capacity is 760, 727, 744, 713, and 575 mAh g^?1 of sulfur at a current density of 80, 160, 320, 800, and 1,600 mA g^?1 based on the sulfur/carbon composite, respectively. What is more, there is almost no decay at the current density of 800 mA g^?1 for 50 cycles and coulombic efficiency remains over 95 %.     

An integrated approach to improve the performance of lean–electrolyte lithium–sulfur batteries

While the sulfur conversion reaction kinetics in Li–S batteries is nowadays improved by the use of appropriate electrocatalysts,it remains a challenge for the batteries to perform well under the lean electrolyte condition where polysulfide shuttle,electrode passivation and the loss of electrolyte due to side reactions,are aggravated.These challenges are addressed in this study by the tandem use of a polysulfide conversion catalyst and a redox–targeting mediator in a gel sulfur cathode.Specifical...