Rational design of MoS_(2) nanosheets decorated on mesoporous hollow carbon spheres as a dual-functional accelerator in sulfur cathode for advanced pouch-type Li–S batteries

Developing sulfur cathodes with high catalytic activity on accelerating the sluggish redox kinetics of lithium polysulfides(Li PSs) and unveiling their mechanisms are pivotal for advanced lithium–sulfur(Li–S)batteries. Herein, MoS2 is verified to reduce the Gibbs free energy for rate-limiting step of sulfur reduction and the dissociation energy of lithium sulfide(Li2 S) for the first time employing theoretical calculations. The Mo S2 nanosheets coated on mesoporous hollow carbon spheres(MHCS) are then reasonably designed as a sulfur host for high-capacity and long-life Li–S battery, in which MHCS can guarantee the high sulfur loading and fast electron/ion transfer. It is revealed that the shuttle effect is efficiently inhibited because of the boosted conversion of Li PSs. As a result, the coin cell based on the MHCS@Mo S2-S cathode exhibits stable cycling performance maintaining 735.7 mAh g^(-1) after 500 cycles at 1.0 C. More importantly, the pouch cell employing the MHCS@Mo S2-S cathodes achieves high specific capacity of1353.2 m Ah g^(-1) and prominent cycle stability that remaining 960.0 m Ah g^(-1) with extraordinary capacity retention of 79.8% at 0.1 C after 170 cycles. Therefore, this work paves a new avenue for developing practical high specific energy and long-life pouch-type Li–S batteries.

Incorporation of layered tin(Ⅳ) phosphate in graphene framework for high performance lithium-sulfur batteries

To anchor the polysulfide and enhance the conversion kinetics of polysulfide to disulfide/sulfide is critical for improving the performance of lithium-sulfur battery.For this purpose,the graphene-supported tin(Ⅳ) phosphate(Sn(HPO_4)_2·H_2 O,SnP) composites(SnP-G) are employed as the novel sulfur hosts in this work.When compared to the graphene-sulfur and carbon-sulfur composites,the SnP-G-sulfur composites exhibit much better cycling performance at 1.0 C over 800 cycles.Meanwhile,the pouch cell fabricated with the SnP-G-sulfur cathodes also exhibits excellent performance with an initial capacity of1266.6 mAh g^(-1)(S) and capacity retention of 76.9% after 100 cycles at 0.1 C.The adsorption tests,density functional theory(DFT) calculations in combination with physical cha racterizations and electrochemical measurements provide insights into the mechanism of capture-accelerated conversion mechanism of polysulfide at the surface of SnP.DFT calculations indicate that the Li-O bond formed between Li atom(from Li_2 S_n,n=1,2,4,6,8) and O atom(from PO_3-OH in SnP) is the main reason for the strong interactions between Li_2 S_n and SnP.As a result,SnP can effectively restrain the shuttle effect and improving the cycling performance of Li-S cell.In addition,by employing the climbing-image nudged elastic band(ciNEB) methods,the energy barrier for lithium sulfide decomposition(charging reaction) on SnP is proved to decrease significantly compared to that on graphene.It can be concluded that SnP is an effective sulfur hosts acting as dual-functional accelerators for the conversion reactions of polysulfude to sulfide(discharging reaction) as well as polysulfide to sulfur(charging reaction).

Lithiated Nafion-garnet ceramic composite electrolyte membrane for solid-state lithium metal battery

Single-ion conducting solid polymer electrolytes are expected to play a vital role in the realization of solid-state Li metal batteries.In this work,a lithiated Nafion(Li-Nafion)-garnet ceramic Li6.25La3 Zr2 Al0.25O12(LLZAO)composite solid electrolyte(CSE)membrane with 30μm thickness was prepared for the first time.By employing X-ray photoelectron spectroscopy and transmission electron microscope,the interaction between LLZAO and Li-Nafion was investigated.It is found that the LLZAO interacts with the Li-Nafion to form a space charge layer at the interface between LLZAO and Li-Nafion.The space charge layer reduces the migration barrier of Li-ions and improves the ionic conductivity of the CSE membrane.The CSE membrane containing 10 wt%LLZAO exhibits the highest ionic conductivity of2.26×10-4 S cm-1 at 30℃among the pristine Li-Nafion membrane,the membrane containing 5 wt%,20 wt%,and 30 wt%LLZAO,respectively.It also exhibits a high Li-ion transference number of 0.92,and a broader electrochemical window of 0-+4.8 V vs.Li+/Li than that of 0-+4.0 V vs.Li+/Li for the pristine Li-Nafion membrane.It is observed that the CSE membrane not only inhibits the growth of Li dendrites but also keeps excellent electrochemical stability with the Li electrode.Benefitting from the above merits,the solid-state LiFePO4/Li cell fabricated with the CSE membrane was practically charged and discharged at 30℃.The cell exhibits an initial reversible discharge specific capacity of 160 mAh g-1 with 97%capacity retention after 100 cycles at 0.2 C,and maintains discharge specific capacity of 126 mAh g-1 after500 cycles at 1 C.The CSE membrane prepared with Li-Nafion and LLZAO is proved to be a promising solid electrolyte for advanced solid-state Li metal batteries.

Polymer-free electrospun separator film comprising silica nanofibers and alumina nanoparticles for Li-ion full cell

A separator film for high-performance Li-ion batteries was prepared by electrospinning. The film had a hybrid morphology of silica nanofibers(SNFs) and alumina nanoparticles(ANPs), with a smooth surface, polymer-free composition, high porosity(79%), high electrolyte uptake(876%), and excellent thermal stability. Contact angle measurements demonstrated the better immersion capability of the SNF-ANP separator film for commercial liquid electrolytes than a commercial CELGARD 2500 separator film. Moreover,compared to the commercial CELGARD 2500 separator, the ionic conductivity of the SNF-ANP separator film was nearly three times higher, the bulk resistance was lower at elevated temperature(120 ℃), the interfacial resistance with lithium metal was lower, and the electrochemical window was wider. Full cells were fabricated to determine the cell performance at room temperature. The specific capacity of the full cell with the SNF-ANP separator film was 165 mAh g-1;the cell was stable for 100 charge/discharge cycles and exhibited a capacity retention of 99.9%. Notably, the electrospun SNF-ANP separator film can be safely used in Li-ion or Li-S rechargeable batteries.

Debating the magnesium-selenium battery technology

Magnesium ion batteries(MIBs)have received tremendous research attention owing to their low cost,dendrite free electroplating,and high theoretical capacities compared with lithium ion batteries(LIBs).Despite these advantages,the launching of MIBs is hindered by sluggish kinetics of the magnesium ions inside the host cathodes.Recently,several magnesium-selenium batteries have been developed to achieve the fast kinetics of magnesium ions inside the selenium-based cathodes.Herein,we have critically reviewed the five-year advancements made in the field of selenium cathode design,selenium loadings,compatible organic and inorganic electrolytes,their resultant reversible capacities,working voltages,cycle life,and specific energies.Selected selenium-based cathodes were critically debated in terms of their electrochemical performance and challenges.At the end of this review article,several irmovative directions are proposed to shed light on future research.c 2020 Published by Elsevier B.V.on behalf of Chongqing University.

A review on lithium-sulfur batteries:Challenge,development,and perspective

Lithium-sulfur(Li-S)battery is recognized as one of the promising candidates to break through the specific energy limitations of commercial lithium-ion batteries given the high theoretical specific energy,environmental friendliness,and low cost.Over the past decade,tremendous progress have been achieved in improving the electrochemical performance especially the lifespan by various strategies mainly concentrated on the sulfur cathodes.In this review,the fundamental electrochemistry of sulfur cathode and lithium anode is revealed to understand the current dilemmas.And the advances achieved through diverse strategies are comprehensively summarized,which involves lithium polysulfides(LiPSs)limitation,sulfur redox reaction regulation and electrocatalysis in sulfur cathode and artificial solid electrolyte interface(SEI),electrolyte design,and structured anode in lithium anode.Additionally,the differences between laboratory level coin cells and actual pouch cells need to be addressed that only few reports on practical Li-S pouch cell are available due to the unexpected problems on both sulfur cathode and lithium anode which are masked at lithium and electrolyte excess.Lastly,the challenges and perspective toward the practical Li-S batteries are also offered.

Li4SiO4-coated LiNi0.5Mn1.5O4 as the high performance cathode materials for lithium-ion batteries

The preparation of Li4SiO4-coated LiNi0.5Mn1.5O4 materials by sintering the SiO2-coated nickel-manganese oxides with lithium salts using abundant and low-cost sodium silicate as the silicon source was reported. The samples were characterized by X-ray diffraction, scanning electron microscopy and transmission electron microscopy. It was found that a uniform and complete SiO2 coating layer could be obtained at a suitable pH value of 10, which transformed to a good LiaSiO4 coating layer afterwards. When used as the cathode materials for lithium-ion batteries, the Li4SiO4-coated LiNi0.5Mn1.5O4 samples deliver a better electrochemical performance in terms of the discharge capacity, rate capability, and cycling stability than that of the pristine material. It can still deliver 111.1 mAh/g at 20 C after 300 cycles, with a retention ratio of 93.1% of the stable capacity, which is far beyond that of the pristine material （101.3 mAh/g, 85.6%）.