Plasma Surface Treatment of Cu Current Collectors for Improving the Electrochemical Performance of Si Anodes.

The practical utilization of Si electrodes is hindered by their substantial volume expansion during alloying and dealloying processes, which causes mechanical damage and separation from Cu current collectors. To alleviate the problem of Si composite detachment from Cu current collectors, the surface of the Cu current collectors is modified using atmospheric oxygen plasma. Plasma treatment improves the wetting ability of the Cu current collectors and, consequently, the coating quality of the Si electrodes. The uniform distribution of the Si electrode components reduces the sheet resistance and improves the adhesion properties of the Si electrodes containing surface-modified Cu current collectors. As a result, the volume expansion of Si during alloying and dealloying is reduced; this results in an excellent rate capability of 1584 mA h g-1 at a current density of 3.6 A g-1 (135% that of bare Cu) and excellent cycle performance of 1545 mA h g-1 after 300 cycles (Si electrodes with bare Cu exhibit 930 mA h g-1). Therefore, the developed plasma treatment method for Cu current collectors is expected to be an economical and efficient approach for improving the Li-ion battery performance.

Synergistically Stabilizing Thin Li Metal through the Formation of a Stable and Highly Conductive Solid Electrolyte Interface and Silver-Lithium Alloy.

In this study, a stable solid electrolyte interface (SEI) and a Ag-Li alloy were formed through a simple slurry coating of silver (Ag) nanoparticles and Li nitrate (LiNO3) on a Li metal surface (AgLN-coated Li). The Ag-Li alloy has a high Li diffusion coefficient, which allowed the inward transfer of Li atoms, thus allowing Li to be deposited below the alloy. Moreover, the highly conductive SEI enabled the fast diffusion of Li ions corresponding to the alloy. This inward transfer resulted in dendrite suppression and improved the Coulombic efficiency (CE). The AgLN-coated Li exhibited an initial capacity retention >81% and CE > 99.7 ± 0.2% over 500 cycles at a discharge capacity of 2.3 mA h cm-2.

Dendrite Suppression by Lithium-Ion Redistribution and Lithium Wetting of Lithium Zeolite Li2(Al2Si4O12) in Liquid Electrolytes.

Lithium metal is considered a next-generation anode material for high-voltage, high-energy-density batteries; however, its commercialization is limited because of dendrite formation during charging, which leads to short-circuiting and fire. Li metal is coated with a lithium zeolite Li2(Al2Si4O12) (bikitaite - BKT) for dendrite suppression. The BKT-coated Li metal anode exhibits enhanced cycle performance for both Li/LMO (over 982 cycles) and Li/Li cells (over 2000 h at 0.52.0 mAh cm-2 and 693 h at 2.0 mAh cm-2). Moreover, the voltage profile of the Li/Li cells deviates from the conventional Li plating behavior. We hypothesize that this is due to the Li wetting of the BKT particles during plating, which leads to the formation of an interconnected three-dimensional (3D) Li network. Furthermore, BKT, a Li conductor, promotes even Li+-ion distribution during plating, resulting in the uniform deposition of Li and, consequently, suppressed dendrite formation. This work provides evidence that BKT can be potentially used in Li metal batteries.

Synergistic Effect of a Dual-Salt Liquid Electrolyte with a LiNO3 Functional Additive toward Stabilizing Thin-Film Li Metal Electrodes for Li Secondary Batteries.

Li metal thickness has been considered a key factor in determining the electrochemical performance of Li metal anodes. The use of thin Li metal anodes is a prerequisite for increasing the energy density of Li secondary batteries intended for emerging large-scale electrical applications, such as electric vehicles and energy storage systems. To utilize thin (20 µm thick) Li metal anodes in Li metal secondary batteries, we investigated the synergistic effect of a functional additive (Li nitrate, LiNO3) and a dual-salt electrolyte (DSE) system composed of Li bis(fluorosulfonyl)imide (LiTFSI) and Li bis(oxalate)borate (LiBOB). By controlling the amount of LiNO3 in DSE, we found that DSE containing 0.05 M LiNO3 (DSE-0.05 M LiNO3) significantly improved the electrochemical performance of Li metal anodes. DSE-0.05 M LiNO3 increased the cycling performance by 146.3% [under the conditions of a 1C rate (2.0 mA cm-2), DSE alone maintained 80% of the initial discharge capacity up to the 205th cycle, whereas DSE-0.05 M LiNO3 maintained 80% up to the 300th cycle] and increased the rate capability by 128.2% compared with DSE alone [the rate capability of DSE-0.05 M LiNO3 = 50.4 mAh g-1, and DSE = 39.3 mAh g-1 under 7C rate conditions (14.0 mA cm-2)]. After analyzing the Li metal surface using scanning electron microscopy and X-ray photoelectron spectroscopy, we were able to infer that the stabilized solid electrolyte interphase layer formed by the combination of LiNO3 and the dual salt resulted in a uniform Li deposition during repeated Li plating/stripping processes.

Preparation and Electrical Properties of Silicone Composite Films Based on Silver Nanoparticle Decorated Multi-Walled Carbon Nanotubes.

The electrical properties of silicone composite films filled with silver (Ag) nanoparticle-decorated multi-walled carbon nanotubes (MWNT) prepared by solution processing are investigated. Pristine MWNT is oxidized and converted to the acyl chloride-functionalized MWNT using thionyl chloride, which is subsequently reacted with amine-terminated poly(dimethylsiloxane) (APDMS). Thereafter, APDMS-modified MWNT are decorated with Ag nanoparticles and then reacted with a poly(dimethylsiloxane) solution to form Ag-decorated MWNT silicone (Ag-decorated MWNT-APDMS/Silicone) composite. The morphological differences of the silicone composites containing Ag-decorated MWNT and APDMS-modified MWNT are observed by transmission electron microscopy (TEM) and the surface conductivities are measured by the four-probe method. Ag-decorated MWNT-APDMS/Silicone composite films show higher surface electrical conductivity than MWNT/silicone composite films. This shows that the electrical properties of Ag-decorated MWNT-APDMS/silicone composite films can be improved by the surface modification of MWNT with APDMS and Ag nanoparticles, thereby expanding their applications.

Nature inspired approach to mimic design for increased specific capacitance as supercapacitor electrodes.

In this study, the experiment was conducted assuming that the citrus fruits were contaminated with bacteria. Herein, orange peels (OP) and lemon peels (LP) can be used as a carbon source and have the advantage of using discarded materials and heteroatoms. Also, the nitrogen heteroatom is introduced by naturally doping the materials with bacteria (Escherichia Coli, E. coli). The as-prepared bacteria doped activated carbon showed an increase in nitrogen content and surface properties which led to an improvement in electrochemical properties. The specific capacitance of bacteria doped OP and LP was 92.4 and 139 Fg-1 compared to the bare samples with a specific capacitance of 60.9 and 49.6 Fg-1 at a current density of 0.2Ag-1 and capacity retention of 129% after 10,000 cycles for the bacteria-doped samples. This process which is simple, cheap, and environmentally friendly can be applied to discarded fruit peels for the fabrication of supercapacitor materials.

Microalgae-Templated Spray Drying for Hierarchical and Porous Fe3O4/C Composite Microspheres as Li-ion Battery Anode Materials.

A method of microalgae-templated spray drying to develop hierarchical porous Fe3O4/C composite microspheres as anode materials for Li-ion batteries was developed. During the spray-drying process, individual microalgae serve as building blocks of raspberry-like hollow microspheres via self-assembly. In the present study, microalgae-derived carbon matrices, naturally doped heteroatoms, and hierarchical porous structural features synergistically contributed to the high electrochemical performance of the Fe3O4/C composite microspheres, enabling a discharge capacity of 1375 mA·h·g-1 after 700 cycles at a current density of 1 A/g. Notably, the microalgal frameworks of the Fe3O4/C composite microspheres were maintained over the course of charge/discharge cycling, thus demonstrating the structural stability of the composite microspheres against pulverization. In contrast, the sample fabricated without microalgal templating showed significant capacity drops (up to ~40% of initial capacity) during the early cycles. Clearly, templating of microalgae endows anode materials with superior cycling stability.

Highly Stable Porous Polyimide Sponge as a Separator for Lithium-metal Secondary Batteries.

To inhibit Li-dendrite growth on lithium (Li)-metal electrodes, which causes capacity deterioration and safety issues in Li-ion batteries, we prepared a porous polyimide (PI) sponge using a solution-processable high internal-phase emulsion technique with a water-soluble PI precursor solution; the process is not only simple but also environmentally friendly. The prepared PI sponge was processed into porous PI separators and used for Li-metal electrodes. The physical properties (e.g., thermal stability, liquid electrolyte uptake, and ionic conductivity) of the porous PI separators and their effect on the Li-metal anodes (e.g., self-discharge and open-circuit voltage properties after storage, cycle performance, rate capability, and morphological changes) were investigated. Owing to the thermally stable properties of the PI polymer, the porous PI separators demonstrated no dimensional changes up to 180 °C. In comparison with commercialized polyethylene (PE) separators, the porous PI separators exhibited improved wetting ability for liquid electrolytes; thus, the latter improved not only the physical properties (e.g., improved the electrolyte uptake and ionic conductivity) but also the electrochemical properties of Li-metal electrodes (e.g., maintained stable self-discharge capacity and open-circuit voltage features after storage and improved the cycle performance and rate capability) in comparison with PE separators.