3D-Printed Thermoplastic Polyurethane Electrodes for Customizable, Flexible Lithium-Ion Batteries with an Ultra-Long Lifetime.

3D printing technology has demonstrated great potential in fabricating flexible and customizable high-performance batteries, which are highly desired in the forthcoming intelligent and ubiquitous energy era. However, a significant performance gap, especially in cycling stability, still exists between the 3D-printed and conventional electrodes, seriously limiting the practical applications of 3D-printed batteries. Here, for the first time, a series of thermoplastic polyurethane (TPU)-based 3D-printed electrodes is developed via fused deposition modeling for flexible and customizable high-performance lithium-ion batteries. The TPU-based electrode filaments in kilogram order are prepared via a facile extrusion method. As a result, the electrodes are well-printed with high dimensional accuracy, flexibility, and mechanical stability. Notably, 3D-printed TPU-LFP electrodes exhibit a capacity retention of 100% after 300 cycles at 1C, which is among the best cycling performance of all the reported 3D-printed electrodes. Such excellent performance is associated with the superb stress cushioning properties of the TPU-based electrodes that can accommodate the volume change during the cycling and thus significantly prevent the collapse of 3D-printed electrode structures. The findings not only provide a new avenue to achieve customizable and flexible batteries but also guide a promising way to erase the performance gap between 3D-printed and conventional lithium-ion batteries.

Small Additives Make Big Differences: A Review on Advanced Additives for High-Performance Solid-State Li Metal Batteries.

Solid-state lithium (Li) metal batteries, represent a significant advancement in energy storage technology, offering higher energy densities and enhanced safety over traditional Li-ion batteries. However, solid-state electrolytes (SSEs) face critical challenges such as lower ionic conductivity, poor stability at the electrode-electrolyte interface, and dendrite formation, potentially leading to short circuits and battery failure. The introduction of additives into SSEs has emerged as a transformative approach to address these challenges. A small amount of additives, encompassing a range from inorganic and organic materials to nanostructures, effectively improve ionic conductivity, drawing it nearer to that of their liquid counterparts, and strengthen mechanical properties to prevent cracking of SSEs and maintain stable interfaces. Importantly, they also play a critical role in inhibiting the growth of dendritic Li, thereby enhancing the safety and extending the lifespan of the batteries. In this review, the wide variety of additives that have been investigated, is comprehensively explored, emphasizing how they can be effectively incorporated into SSEs. By dissecting the operational mechanisms of these additives, the review hopes to provide valuable insights that can help researchers in developing more effective SSEs, leading to the creation of more efficient and reliable solid-state Li metal batteries.

Hybrid Artificial Solid Electrolyte Interphase with Dendrite-Free Lithium Deposition and High Ion Transport Kinetics.

Interfacial issues and dendritic Li deposition in lithium metal batteries (LMBs) hamper the practical application of liquid or solid-state cells. Here, a hybrid solid electrolyte interphase (SEI), based on hydroxyl-functionalized boron nitride (BN) nanosheets and poly(vinyl alcohol), is designed to solve the unstable nature of the Li anode-electrolyte interface. Rather than acquiring a rich Li halide environment through intense electrolyte decomposition, the hybrid SEI effectively regulates electrolyte decomposition and guarantees uniform Li plating via boosting interfacial Li+ ion transport at the interface. The Li+ ion boosting kinetics were deeply analyzed using simulations and spectroscopic analysis. It is revealed that the hydroxyl-functionalized BN can decrease kinetic energy barriers for Li+ ions and strongly holds TFSI- ions, thereby ensuring faster Li+ ion migration between electrodes and electrolytes. Tailoring the interfacial Li+ ion dynamics with hybrid SEI renders the Li transference number enhancement from 0.391 to 0.562 and 0.178 to 0.327 in liquid and solid-state cells, respectively. Moreover, Li symmetric cells with hybrid SEI exhibit an ultrahigh stability over 3500 h at 2 mA cm-2 with 2 mA h cm-2, along with the improved solid-state LMB performances. Our results suggest increasing Li+ ion transport at the interface is an alternative to resolve Li anode issues.

An Ultra-Long-Life Flexible Lithium-Sulfur Battery with Lithium Cloth Anode and Polysulfone-Functionalized Separator.

Flexible and high-performance batteries are urgently required for powering flexible/wearable electronics. Lithium-sulfur batteries with a very high energy density are a promising candidate for high-energy-density flexible power source. Here, we report flexible lithium-sulfur full cells consisting of ultrastable lithium cloth anodes, polysulfone-functionalized separators, and free-standing sulfur/graphene/boron nitride nanosheet cathodes. The carbon cloth decorated with lithiophilic three-dimensional MnO2 nanosheets not only provides the lithium anodes with an excellent flexibility but also limits the growth of the lithium dendrites during cycling, as revealed by theoretical calculations. Commercial separators are functionalized with polysulfone (PSU) via a phase inversion strategy, resulting in an improved thermal stability and smaller pore size. Due to the synergistic effect of the PSU-functionalized separators and boron nitride-graphene interlayers, the shuttle of the polysulfides is significantly inhibited. Because of successful control of the shuttle effect and dendrite formation, the flexible lithium-sulfur full cells exhibit excellent mechanical flexibility and outstanding electrochemical performance, which shows a superlong lifetime of 800 cycles in the folded state and a high areal capacity of 5.13 mAh cm-2. We envision that the flexible strategy presented herein holds promise as a versatile and scalable platform for large-scale development of high-performance flexible batteries.

A Self-Healing Amalgam Interface in Metal Batteries.

Poor cyclability and safety concerns caused by the uncontrollable dendrite growth and large interfacial resistance severely restrict the practical applications of metal batteries. Herein, a facile, universal strategy to fabricate ceramic and glass phase compatible, and self-healing metal anodes is proposed. Various amalgam-metal anodes (Li, Na, Zn, Al, and Mg) show a long cycle life in symmetric cells. It has been found that liquid Li amalgam shows a complete wetting with the surface of lanthanum lithium titanate electrolyte and a glass-phase solid-state electrolyte. The interfacial compatibility between the lithium metal anode and solid-state electrolyte is dramatically improved by using an in situ regenerated amalgam interface with high electron/ion dual-conductivity, obviously decreasing the anode/electrolyte interfacial impedance. The lithium-amalgam interface between the metal anode and electrolyte undergoes a reversible isothermal phase transition between solid and liquid during the cycling process at room temperature, resulting in a self-healing surface of metal anodes.

Synthesis and loading-dependent characteristics of nitrogen-doped graphene foam/carbon nanotube/manganese oxide ternary composite electrodes for high performance supercapacitors.

The ternary composite electrodes, nitrogen-doped graphene foam/carbon nanotube/manganese dioxide (NGF/CNT/MnO2), have been successfully fabricated via chemical vapor deposition (CVD) and facile hydrothermal method. The morphologies of the MnO2 nanoflakes presented the loading-dependent characteristics and the nanoflake thickness could also be tuned by MnO2 mass loading in the fabrication process. The correlation between their morphology and electrochemical performance was systematically investigated by controlling MnO2 mass loading in the ternary composite electrodes. The electrochemical properties of the flexible ternary electrode (MnO2 mass loading of 70%) exhibited a high areal capacitance of 3.03F/cm2 and a high specific capacitance of 284F/g at the scan rate of 2mV/s. Moreover, it was interesting to find that the capacitance of the NGF/CNT/MnO2 composite electrodes showed a 51.6% increase after 15,000 cycles. The gradual increase in specific capacitance was due to the formation of defective regions in the MnO2 nanostructures during the electrochemical cycles of the electrodes, which further resulted in increased porosity, surface area, and consequently increased electrochemical capacity. This work demonstrates a rarely reported conclusion about loading-dependent characteristics for the NGF/CNT/MnO2 ternary composite electrodes. It will bring new perspectives on designing novel ternary or multi-structure for various energy storage applications.

Human-like collagen protein-coated magnetic nanoparticles with high magnetic hyperthermia performance and improved biocompatibility.

Human-like collagen (HLC)-coated monodispersed superparamagnetic Fe3O4 nanoparticles have been successfully prepared to investigate its effect on heat induction property and cell toxicity. After coating of HLC, the sample shows a faster rate of temperature increase under an alternating magnetic field although it has a reduced saturation magnetization. This is most probably a result of the effective heat conduction and good colloid stability due to the high charge of HLC on the surface. In addition, compared with Fe3O4 nanoparticles before coating with HLC, HLC-coated Fe3O4 nanoparticles do not induce notable cytotoxic effect at higher concentration which indicates that HLC-coated Fe3O4 nanoparticles has improved biocompatibility. Our results clearly show that Fe3O4 nanoparticles after coating with HLC not only possess effective heat induction for cancer treatment but also have improved biocompatibility for biomedicine applications.