Ge Li

The development of high-energy-density anodes capable of withstanding fast-charging conditions remains a significant challenge for lithium-ion batteries. Silicon monoxide (SiO_x) is a promising candidate, yet its performance intrinsically depends on the structure of the lithium silicate matrix formed during the initial lithiation. Herein, we demonstrate that the lithiation method, chemical versus electrochemical, serves as a powerful tool for the precise phase engineering of this silicate component. We selectively synthesized Li₂Si₂O₅, Li₂SiO₃, and Li₄SiO₄, establishing that the [NBO]/[Si] ratio is the key descriptor for Li-ion transport kinetics. Multiscale simulations confirm that nonbridging oxygen (NBO) sites provide low-energy migration pathways, whereas bridging oxygen (BO) sites impede ion mobility. The electrochemically derived Li₄SiO₄ phase, which possesses the highest [NBO]/[Si] ratio, consequently enables a superior fast-charging performance. Practical validation using 2-Ah pouch cells demonstrates 85% capacity retention after 300 cycles at 4C (15-min charging). This work establishes lithiation engineering as a fundamental strategy for developing high-performance SiO_x anodes, transforming it from a simple pretreatment into a critical design parameter for fast-charging batteries.

The transition from fossil fuels to environmentally friendly renewable energy sources is crucial for achieving global initiatives such as the carbon peak and carbon neutrality. The use of secondary batteries and supercapacitors based on electrochemical energy storage principles provides high energy density, conversion efficiency, and rapid response times, offering essential solutions for stabilizing and ensuring the reliability of energy supply from renewable sources despite their intermittency. In recent years, increased demands for higher energy density, improved rate performance, longer cycle life, enhanced safety, and cost-effectiveness have driven researchers to delve deeper into electrode materials, electrolytes, and storage mechanisms in secondary batteries. This effort has led to various modification techniques and rapid advancements in next-generation secondary batteries, which are presented in this roadmap. The design principles, research advancements, and failure mechanisms of component materials of high-energy-density lithium-ion batteries, sodium/potassium-ion batteries, multivalent metal-ion batteries, alkali metal batteries, metal-sulfur batteries, metal-air batteries, solid-state batteries, redox flow batteries, and supercapacitors are systematically summarized. More importantly, the potential future solutions are suggested to narrow the gap between the current energy storage systems and future demands of practical grid-scale energy storage, thereby promoting their widespread application.

Lenvatinib (LVN) is a potentially effective multiple-targeted receptor tyrosine kinase inhibitor approved for treating hepatocellular carcinoma, metastatic renal cell carcinoma and thyroid cancer. Nonetheless, poor pharmacokinetic properties including poor water solubility and rapid metabolic, complex tumor microenvironment, and drug resistance have impeded its satisfactory therapeutic efficacy. This article comprehensively reviews the uses of nanotechnology in LVN to improve antitumor effects. With the characteristic of high modifiability and loading capacity of the nano-drug delivery system, an active targeting approach, controllable drug release, and biomimetic strategies have been devised to deliver LVN to target tumors in sequence, compensating for the lack of passive targeting. The existing applications and advances of LVN in improving therapeutic efficacy include improving longer-term efficiency, achieving higher efficiency, combination therapy, tracking and diagnosing application and reducing toxicity. Therefore, using multiple strategies combined with photothermal, photodynamic, and immunoregulatory therapies potentially overcomes multi-drug resistance, regulates unfavorable tumor microenvironment, and yields higher synergistic antitumor effects. In brief, the nano-LVN delivery system has brought light to the war against cancer while at the same time improving the antitumor effect. More intelligent and multifunctional nanoparticles should be investigated and further converted into clinical applications in the future.

Safety concerns related to the abuse operation and thermal runaway are impeding the large-scale employment of high-energy-density rechargeable lithium batteries. Here, we report that by incorporating phosphorus-contained functional groups into a hydrocarbon-based polymer, a smart risk-responding polymer is prepared for effective mitigation of battery thermal runaway. At room temperature, the polymer is (electro)chemically compatible with electrodes, ensuring the stable battery operation. Upon thermal accumulation, the phosphorus-containing radicals spontaneously dissociate from the polymer skeleton and scavenge hydrogen and hydroxyl radicals to terminate the exothermic chain reaction, suppressing thermal generation at an early stage. With the smart risk-responding strategy, we demonstrate extending the time before thermal runaway for a 1.8-Ah Li-ion pouch cell by 100% (~9 hours) compared with common cells, creating a critical time window for safety management. The temperature-triggered automatic safety-responding strategy will improve high-energy-density battery tolerance against thermal abuse risk and pave the way to safer rechargeable batteries.

Microsized SiO_x has been vigorously investigated as an advanced anode material for next-generation lithium-ion batteries. However, its practical application is seriously hampered by its huge volume variation during the repeated (de)lithiation process, which destroys the microparticle structure and results in rapid capacity fading. Herein, we propose the usage of trans-difluoroethylene carbonate (DFEC) as an electrolyte additive to maintain the structural integrity of microsized SiO_x with a uniform carbon layer (SiO_x@C). Compared with ethylene carbonate and fluoroethylene carbonate, DFEC has lower lowest unoccupied molecular orbital energy and higher reduction potential, which is easily reduced and promotes the in situ formation of a more stable LiF-rich solid electrolyte interphase (SEI) on the surface of anode materials. The LiF-rich SEI exhibits enhanced mechanical rigidity and ionic conductivity, thus enabling the microsized SiO_x@C anodes’ excellent lithium storage stability and high average Coulombic efficiency.

Carbon-coated SiOx microparticles (SiOx/C) demonstrate attractive potential for anode use in high energy density lithium-ion batteries due to high capacity and proper cycling stability. However, the excessive irreversible consumption of Li ions during the initial cycling remains a serious challenge arising from the limited lithium in full-cells. Here, we enable SiOx/C anode with high initial Coulombic efficiency by chemical pre-lithiation strategy. The lithium silicate is uniformly pre-generated in SiOx microparticles which could effectively counteract the irreversible consumption of Li ions and avoid the complicate pre-lithiation process. Moreover, this strategy guarantees the structure integrity and processability of anode materials because of the homogeneous Li-organic complex solution pre-lithiation and high-temperature calcination process. The obtained SiOx/C microparticles can be applied as anode materials by directly mixing with commercial graphite which demonstrate proper specific capacity, high initial Coulombic efficiency and excellent cycling performance. Furthermore, the pouch-cells using LiNi0.8Co0.1Mn0.1O2 cathodes and the as-prepared anodes exhibit high energy density (301 Wh kg-1) and satisfactory cycling stability (93.3% capacity retention after 100 cycles).

Silicon-based electrodes are promising and appealing for futuristic Li-ion batteries because of their high theoretical specific capacity. However, massive volume change of silicon upon lithiation and delithiation, accompanied by continual formation and destruction of the solid–electrolyte interface (SEI), leads to low Coulombic efficiency. Prelithiation of Si-based anode is regarded as an effective way for compensating for the loss of Li⁺ in the first discharging process. Here, a high-performance lithiated SiO_x anode was prepared by using a controllable, efficient, and novel prelithiation strategy. The lithiation of SiO_x is homogeneous and efficient in bulk due to well-improved Li⁺ diffusion in SiO_x. Moreover, the in situ formed SEI during the process of prelithiation reduces the irreversible capacity loss in the first cycle and thus improves the initial Coulombic efficiency (ICE). Half-cells and full cells based on the as-prepared lithiated SiO_x anode prominently increase the ICE from 79 to 89% and 68 to 87%, respectively. It is worth mentioning that the homogeneously lithiated SiO_x anode achieves stable 200 cycles in NCM622//SiO_x coin full cells. These exciting results provide applicable prospects of lithiated SiO_x anode in the next-generation high-energy-density Li-ion batteries.