Engineering Moderately Lithiophilic Paper-Based Current Collectors with Variable Solid Electrolyte Interface Films for Anode-Free Lithium Batteries.

Compared to traditional lithium metal batteries, anode-free lithium metal batteries use bare current collectors as an anode instead of Li metal, making them highly promising for mass production and achieving high-energy density. The current collector, as the sole component of the anode, is crucial in lithium deposition-stripping behavior and greatly impacts the rate of Li depletion from the cathode. In this study, to investigate the lithiophilicity effect of the current collector on the solid electrolyte interface (SEI) film construction and cycling performance of anode-free lithium batteries, various lightweight paper-based current collectors were prepared by electroless plating Cu and lipophilic Ag on low-dust paper (LDP). The areal densities of the as-prepared LDP@Cu, LDP@Cu-Ag, and LDP@Ag were approximately 0.33 mg cm-2. The use of lipophilic Ag-coated collectors with varying loadings allowed for the regulation of lipophilicity. The impacts of these collectors on the distribution of SEI components and Li depletion rate in common electrolytes were investigated. The findings suggest that higher loadings of lipophilic materials, such as Ag, on the current collector increase its lipophilicity but also lead to significant Li depletion during the cycling process in full-cell anode-free Li metal batteries. Thus, moderately lithiophilic current collectors, such as LDP@Cu-Ag, show more potential for Li deposition and striping and stable SEI with a low speed of Li depletion.

The Impact of Oxygen Content in O-Doped MoS2 on the Kinetics of Polysulfide Conversion in Li-S Batteries.

Polysulfide shuttle and sluggish sulfur redox kinetics remain key challenges in lithium-sulfur batteries. Previous researches have shown that introducing oxygen into transition metal sulfides helps to capture polysulfides and enhance their conversion kinetics. Based on this, further investigations are conducted to explore the impact of oxygen doping levels on the physical-chemical properties and electrocatalytic performance of MoS2. The findings reveal that MoS2 doped with high-content oxygen exhibits enhanced conductivity and polysulfides conversion kinetics compared to MoS2 with low-content oxygen doping, which can be attributed to the alteration of crystal structure from 2H-phase to the 1T-phase, the introduction of increased Li-O interactions, and the effect of defects resulting from high-oxygen doping. Consequently, the lithium-sulfur batteries using high-oxygen doped MoS2 as a catalyst deliver a high discharge capacity of 1015 mAh g-1 at 0.25C and maintain 78.5% capacity after 300 more cycles. Specifically, lithium-sulfur batteries employing paper-based electrodedemonstrate an areal capacity of 3.91 mAh cm-2 at 0.15C, even with sulfur loading of 4.1 mg cm-2 and electrolyte of 6.7 µL mg-1. These results indicate that oxygen doping levels can modify the properties of MoS2, and high-oxygen doped MoS2 shows promise as an efficient catalyst for lithium-sulfur batteries.

Self-Supporting Flexible Paper-Based Electrode Reinforced by Gradient Network Structure.

At present, the self-supporting paper-based electrode has some problems, such as low mechanical strength and insufficient flexibility, which restrict its application in flexible electronics. In this paper, FWF is used as the skeleton fiber, and the contact area and the number of hydrogen bonds of the fiber are increased by grinding the fiber and adding nanofibers to bridge it, and a level three gradient enhanced skeleton support network structure is constructed, which effectively improves the mechanical strength and foldability of the paper-based electrodes. The tensile strength of FWF15-BNF5 paper-based electrode is 7.4 MPa, the elongation at break is increased to 3.7%, the electrode thickness is as low as 66 µm, the electrical conductivities is 5.6 S cm-1, and the contact angle to electrolyte as low as 45°, which has excellent electrolyte wettability, flexibility, and foldability. After three-layer superimposed rolling, the discharge areal capacity reached 3.3 mAh cm-2 and 2.9 mAh cm-2 at the rate of 0.1 C and 1.5 C, respectively, which was superior to the commercial LFP electrode, it had good cycle stability, and the areal capacity was 3.0 mAh cm-2 and 2.8 mAh cm-2 after 100 cycles at the rate of 0.3 C and 1.5 C.

High-Density Oxygen Doping of Conductive Metal Sulfides for Better Polysulfide Trapping and Li2 S-S8 Redox Kinetics in High Areal Capacity Lithium-Sulfur Batteries.

Exploring new materials and methods to achieve high utilization of sulfur with lean electrolyte is still a common concern in lithium-sulfur batteries. Here, high-density oxygen doping chemistry is introduced for making highly conducting, chemically stable sulfides with a much higher affinity to lithium polysulfides. It is found that doping large amounts of oxygen into NiCo2 S4 is feasible and can make it outperform the pristine oxides and natively oxidized sulfides. Taking the advantages of high conductivity, chemical stability, the introduced large Li-O interactions, and activated Co (Ni) facets for catalyzing Sn 2- , the NiCo2 (O-S)4 is able to accelerate the Li2 S-S8 redox kinetics. Specifically, lithium-sulfur batteries using free-standing NiCo2 (O-S)4 paper and interlayer exhibit the highest capacity of 8.68 mAh cm-2 at 1.0 mA cm-2 even with a sulfur loading of 8.75 mg cm-2 and lean electrolyte of 3.8 µL g-1 . The high-density oxygen doping chemistry can be also applied to other metal compounds, suggesting a potential way for developing more powerful catalysts towards high performance of Li-S batteries.