Lithium‐ion batteries (LIBs) are one of the most exciting inventions of the 20th century and have been widely employed in modern society. LIBs have powered many of our electronics, such as laptop computers, smartphones, and even large‐scale energy storage systems. With the development of modern technology, next‐generation LIBs with higher energy density are in demand. A number of electrode materials with high theoretical capacity, including Sn, Si, Li metal anode, and S cathode materials, have been explored. Nevertheless, they usually suffer from structural or interface failure during cycling, limiting their practical application. Ga‐based liquid metals (LMs) possess self‐healing capability, fluidity, and metallic advantages so they have been employed as self‐healing skeletons or interfacial protective layers to minimize the negative impact of volume expansion or dendritic growth on the electrode materials. Herein, the features of Ga‐based LMs are briefly discussed to indicate their potential for battery systems. In addition, recent developments on Ga‐based LMs applied in LIBs have been summarized, including from the aspects of anodes, cathodes, and electrolytes. Finally, future opportunities and challenges for the development of Ga‐based LMs in LIBs are highlighted.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/idm2.12042

Gallium‐based liquid metals for lithium‐ion batteries

Li metal has been recognized as the most promising anode materials for next-generation high-energy-density batteries, however, the inherent issues of dendrite growth and huge volume fluctuations upon Li plating/stripping normally result in fast capacity fading and safety concerns. Functionalized Cu current collectors have so far exhibited significant regulatory effects on stabilizing Li metal anodes (LMAs), and hold a great practical potential owing to their easy fabrication, low-cost and good compatibility with the existing battery technology. In this review, a comprehensive overview of Cu-based current collectors, including planar modified Cu foil, 3D architectured Cu foil and nanostructured 3D Cu substrates, for Li metal batteries is provided. Particularly, the design principles and strategies of functionalized Cu current collectors associated with their functionalities in optimizing Li plating/stripping behaviors are discussed. Finally, the critical issues where there is incomplete understanding and the future research directions of Cu current collectors in practical LMAs are also prospected. This review may shed light on the critical understanding of current collector engineering for high-energy-density Li metal batteries. 

https://www.sciopen.com/article_pdf/1603591289620283394.pdf

Present and future of functionalized Cu current collectors for stabilizing lithium metal anodes

3D Cu current collectors have been demonstrated to improve the cycling stability of Li metal anodes, however, the role of their interfacial structure for Li deposition pattern has not been investigated thoroughly. Herein, a series of 3D integrated gradient Cu-based current collectors are fabricated by the electrochemical growth of CuO nanowire arrays on Cu foil (CuO@Cu), where their interfacial structures can be readily controlled by modulating the dispersities of the nanowire arrays. It is found that the interfacial structures constructed by sparse and dense dispersion of CuO nanowire arrays are both disadvantageous for the nucleation and deposition of Li metal, consequently fast dendrite growth. In contrast, a uniform and appropriate dispersity of CuO nanowire arrays enables stable bottom Li nucleation associated with smooth lateral deposition, affording the ideal bottom-up Li growth pattern. The optimized CuO@Cu-Li electrodes exhibit a highly reversible Li cycling including a coulombic efficiency of up to ≈99% after 150 cycles and a long-term lifespan of over 1200 h. When coupling with LiFePO4 cathode, the coin and pouch full-cells deliver outstanding cycling stability and rate capability. This work provides a new insight to design the gradient Cu current collectors toward high-performance Li metal anodes.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/advs.202301288

Integrated Gradient Cu Current Collector Enables Bottom-Up Li Growth for Li Metal Anodes: Role of Interfacial Structure.

Li metal has been considered as a potential anode candidate for next‐generation high‐energy Li‐metal batteries, even though the uncontrollable growth of Li dendrites shortens their cycling lifespan. Herein, a reliable and dendrite‐free Li‐metal anode is fabricated via inducing chemical confinement based on an atomic layer deposited lithiophilic ZnO in situ generating LiZn/Li2O arrays. In a configuration, the arrays consisting of uniformly distributed LiZn and Li2O phases, the lithiophilic Li2O phases with favorable Li diffusion barrier guarantee the preferential Li nucleation and prevent the Li diffusion to some sites with uneven charge accumulation. Furthermore, these functional LiZn/Li2O configurations with satisfied localized free electron distribution can effectively decompose the Li clusters to prevent Li aggregation. Meanwhile, the electron‐conductive LiZn phases ensure efficient electron transfer throughout the configuration. Therefore, the LiZn/Li2O‐derived chemical confinement enables uniform Li deposition. Consequently, the as‐prepared Li‐metal anode presents an overpotential <45 mV at 15 mA cm−2 in the symmetrical cells. Moreover, the preferable cycling stability and rate capability are delivered by the as‐assembled cells with a LiNi0.6Co0.2Mn0.2O2 (NCM622) cathode. It is believed that the strategy proposed here can be also beneficial to other effective chemical confinement systems for fabricating high‐performance Li metal anode.

LiZn/Li2O Induced Chemical Confinement Enabling Dendrite‐Free Li‐Metal Anode

Metallic Na is a promising metal anode for large-scale energy storage. Nevertheless, unstable solid electrolyte interphase (SEI) and uncontrollable Na dendrite growth lead to disastrous short circuit and poor cycle life. Through phase field and ab initio molecular dynamics simulation, we first predict that the sodium bromide (NaBr) with the lowest Na ion diffusion energy barrier among sodium halogen compounds (NaX, X=F, Cl, Br, I) is the ideal SEI composition to induce the spherical Na deposition for suppressing dendrite growth. Then, 1,2-dibromobenzene (1,2-DBB) additive is introduced into the common fluoroethylene carbonate-based carbonate electrolyte (the corresponding SEI has high mechanical stability) to construct a desirable NaBr-rich stable SEI layer. When the Na||Na3 V2 (PO4 )3 cell utilizes the electrolyte with 1,2-DBB additive, an extraordinary capacity retention of 94 % is achieved after 2000 cycles at a high rate of 10 C. This study provides a design philosophy for dendrite-free Na metal anode and can be expanded to other metal anodes.

Designing Solid Electrolyte Interfaces towards Homogeneous Na Deposition: Theoretical Guidelines for Electrolyte Additives and Superior High-Rate Cycling Stability.

Lithium metal is an ideal anode for next‐generation high‐energy‐density batteries. However, lithium dendrite growth has impeded its commercial application. Herein, fabricating Li‐based ultrathin alloys with electronic localization and high surface work function via depositing Bi, Al, or Au metals on the surface of copper foil for in situ alloying with lithium is proposed. It is discovered that the electronic localization can induce self‐smoothing effect of Li ions, as a result, significantly suppressing the growth of dendritic lithium. Meanwhile, the high surface work function can effectively alleviate side reactions between the electrolyte and lithium. With the as‐obtained ultrathin alloys as anodes, excellent cycling performance is achieved. The half cells run stably after more than 120 cycles under high capacity of 4 mAh cm−2. The S||Bi/Cu‐Li full cell delivers a specific capacity of 736 mAh g−1 after 200 cycles. This work provides a new strategy for fabricating long‐life and high‐capacity lithium batteries.

Electronic Localization Derived Excellent Stability of Li Metal Anode with Ultrathin Alloy

Co magnetic films are widely used in high-frequency magnetic recording and vertical magnetic recording due to their high saturation magnetization and magnetocrystalline anisotropy. In this work, ferromagnetic Co magnetic films were prepared on copper substrate by vacuum evaporation combined with heat treatment (H2 atmosphere), to investigate the impact of film thickness and annealing temperature on microstructure and magnetic properties. The results show that with the increase in annealing temperature, the Co thin film physical phase does not change significantly, the crystallinity increases, and the grain size increases, which is consistent with the results obtained from the SEM morphology map of the sample surface, leading to an increase in coercivity. By annealing experiments (atmospheric atmosphere) on Co magnetic films with and without an Al protective layer, as shown by scanning electron microscopy microscopic characterization results, it was verified that the Al layer can protect the inner Co layer from oxidation. As the film thickness increases from 10 to 300 nm, the magnetic properties of Co films change significantly. The saturation magnetization gradually increases from 0.89 to 5.21 emu/g, and the coercivity increases from 124.3 to 363.8 Oe. The remanence ratio of the 10 nm magnetic film is 0.82, which is much higher than the film remanence ratio of 0.46 at 50 nm. This is because when the thickness of the film is between 10 and 50 nm, the magnetic moments partially deviate from the in-plane direction, and the out-of-plane component reduces the film remanence ratio. This study shows that optimizing annealing temperature and film thickness can effectively control the structure and magnetic properties of Co magnetic films, which is of great significance for the development of the magnetic recording field.

Structure and Performance Optimization of Co Magnetic Thin Films Deposited by Vacuum Evaporation Coating

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Electronic Localization Derived Excellent Stability of Li Metal Anode with Ultrathin Alloy

Structure and Performance Optimization of Co Magnetic Thin Films Deposited by Vacuum Evaporation Coating