Strategies toward High‐Loading Lithium–Sulfur Battery

A polymer sponge with dual absorption of mechanical and electromagnetic energy.

A high sulfur loading is an essential prerequisite for the practical application of lithium–sulfur batteries. However, it will inevitably exacerbate the shuttling effect and slow down the polysulfide conversion kinetics. To obtain desirable electrochemical performance at a high level of sulfur loading, the adsorption and catalysis dual strategies are widely reported to solve the severe shuttling effect and sluggish reaction kinetics issues. This review mainly summarizes the research on lithium–sulfur batteries with a high sulfur loading (>5 mg cm–2) based on adsorption–catalysis dual promotion strategies. Specifically, we review the principle and technical challenges for lithium–sulfur batteries and recent advancements in electrode materials with adsorption and catalysis design, as well as the potential approaches and suggestions for constructing next-generation lithium–sulfur batteries at a high level of sulfur loading. This review will provide practical guidance for lithium–sulfur batteries with high energy density and power density under a high sulfur loading and offer a better reference for researchers to choose adsorbents and catalysts. 

Strategies toward High-Loading Lithium–Sulfur Batteries

Battery materials as emerging capacitive deionization electrodes for desalination have better salt removal capacities than traditional carbon-based materials. LiMn2O4, a widely used cathode material, is difficult to utilize as a deionization electrode due to its structural instability upon cycling and Mn dissolution in aqueous-based electrolytes. Herein, a facile and low-cost ball-milling routine was proposed to prepare a LiMn2O4 material with highly exposed (111) facets. The prepared electrode exhibited relatively low dissolution of Mn during cycling, which shows its long cycle stability. In the hybrid capacitive deionization system, the LiMn2O4/C electrode delivered a high desalination capacity of 117.3 mg g−1 without obvious capacity decay at a voltage of 1.0 V with a 20 mM initial salt concentration. In addition, the exposed (111) facets significantly alleviated Mn ion dissolution, which also enhanced the structural steadiness. 

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Facet-Controlled LiMn2O4/C as Deionization Electrode with Enhanced Stability and High Desalination Performance

Being considered as a promising anode material for next‐generation lithium‐ion batteries, silicon oxide (SiOx) suffers from low initial coulombic eﬃciency and unstable solid–electrolyte interphase (SEI), which hinder its commercial use. To address these issues, herein, an optimized chemical prelithiation method is developed using a molecularly engineered lithium–biphenyl‐type complex, which facilitates improved prelithiation efficiency. More importantly, owing to the reaction between the prelithiation agent and sodium carboxymethyl cellulose binder, a stable artificial SEI layer with hard inorganic particles embedded in soft organic matrix can be preformed on the surface of the SiOx anode after prelithiation. The preformed SEI layer remains stable during long‐term cycling, contributing to significant improvement of capacity retention (87.4%) over pristine SiOx (68.6%) after 100 cycles at 0.2 C. Through demonstrating a hitherto unknown interfacial constructing strategy for SiOx, this study provides a fresh perspective on realizing high‐capacity Si‐based anodes.

Constructing a Robust Solid–Electrolyte Interphase Layer via Chemical Prelithiation for High‐Performance SiOx Anode

Thermal insulation under extreme conditions requires materials that can withstand complex thermomechanical stress and retain excellent thermal insulation properties at temperatures exceeding 1,000 degrees Celsius1-3. Ceramic aerogels are attractive thermal insulating materials; however, at very high temperatures, they often show considerably increased thermal conductivity and limited thermomechanical stability that can lead to catastrophic failure4-6. Here we report a multiscale design of hypocrystalline zircon nanofibrous aerogels with a zig-zag architecture that leads to exceptional thermomechanical stability and ultralow thermal conductivity at high temperatures. The aerogels show a near-zero Poisson's ratio (3.3 × 10-4) and a near-zero thermal expansion coefficient (1.2 × 10-7 per degree Celsius), which ensures excellent structural flexibility and thermomechanical properties. They show high thermal stability with ultralow strength degradation (less than 1 per cent) after sharp thermal shocks, and a high working temperature (up to 1,300 degrees Celsius). By deliberately entrapping residue carbon species in the constituent hypocrystalline zircon fibres, we substantially reduce the thermal radiation heat transfer and achieve one of the lowest high-temperature thermal conductivities among ceramic aerogels so far-104 milliwatts per metre per kelvin at 1,000 degrees Celsius. The combined thermomechanical and thermal insulating properties offer an attractive material system for robust thermal insulation under extreme conditions. 

/pdf/hypocrystalline-ceramic-aerogels-for-thermal-insulation-at-1wuicd9b.pdf

Hypocrystalline ceramic aerogels for thermal insulation at extreme conditions

Abstract Silicon monoxide (SiO) is an attractive anode material for next-generation lithium-ion batteries for its ultra-high theoretical capacity of 2680 mAh g −1 . The studies to date have been limited to electrodes with a relatively low mass loading (&lt; 3.5 mg cm −2 ), which has seriously restricted the areal capacity and its potential in practical devices. Maximizing areal capacity with such high-capacity materials is critical for capitalizing their potential in practical technologies. Herein, we report a monolithic three-dimensional (3D) large-sheet holey graphene framework/SiO (LHGF/SiO) composite for high-mass-loading electrode. By specifically using large-sheet holey graphene building blocks, we construct LHGF with super-elasticity and exceptional mechanical robustness, which is essential for accommodating the large volume change of SiO and ensuring the structure integrity even at ultrahigh mass loading. Additionally, the 3D porous graphene network structure in LHGF ensures excellent electron and ion transport. By systematically tailoring microstructure design, we show the LHGF/SiO anode with a mass loading of 44 mg cm −2 delivers a high areal capacity of 35.4 mAh cm −2 at a current of 8.8 mA cm −2 and retains a capacity of 10.6 mAh cm −2 at 17.6 mA cm −2 , greatly exceeding those of the state-of-the-art commercial or research devices. Furthermore, we show an LHGF/SiO anode with an ultra-high mass loading of 94 mg cm −2 delivers an unprecedented areal capacity up to 140.8 mAh cm −2 . The achievement of such high areal capacities marks a critical step toward realizing the full potential of high-capacity alloy-type electrode materials in practical lithium-ion batteries. 

/pdf/a-silicon-monoxide-lithium-ion-battery-anode-with-ultrahigh-2mx51p54.pdf

A Silicon Monoxide Lithium-Ion Battery Anode with Ultrahigh Areal Capacity

/pdf/a-silicon-monoxide-lithium-ion-battery-anode-with-ultrahigh-25gjunzi.pdf

Shubin Fu

Papers

Hypocrystalline ceramic aerogels for thermal insulation at extreme conditions

A Silicon Monoxide Lithium-Ion Battery Anode with Ultrahigh Areal Capacity

A Silicon Monoxide Lithium-Ion Battery Anode with Ultrahigh Areal Capacity

Defect-Mediated Work Function Regulation in Graphene Film for High-Performing Triboelectric Nanogenerators

Carbonaceous ceramic nanofibrous aerogels for high-temperature thermal superinsulation