Li metal as an ideal anode material meets the requirements of state-of-the-art secondary batteries. However, the dendrite growth of Li causes safety concerns and results in a low coulombic efficiency, which has significantly restricted the commercial applications of Li secondary batteries. Owing to the intrinsic limitations of even the most advanced experimental and computational techniques, a mechanistic understanding of Li deposition (growth) on the atomic scale is lacking.Here, we construct a Li potential model by machine learning with an accuracy of quantum mechanical computations. Our molecular dynamics simulations based on this potential model reveal two self-healing mechanisms in a large Li metal system, surface self-healing and bulk self-healing, and identify three Li dendrite morphologies in different conditions, "needle," "mushroom," and "hemisphere." We finally propose the concepts of local current density and variance of local current density as a supplement to critical current density to determine the probability of self-healing triggered.

Aqueous zinc‐ion batteries (ZIBs) have been extensively studied due to their inherent safety and high energy density for large‐scale energy storage. However, the practical application is significantly limited by the growing Zn dendrites on metallic Zn anode during cycling. Herein, an environmental biomolecular electrolyte additive, fibroin (FI), is proposed to guide the homogeneous Zn deposition and stabilize Zn anode. This work demonstrates that the FI molecules with abundant electron‐rich groups (NH, OH, and CO) can anchor on Zn anode surface to provide more nucleation sites and suppress the side reactions, and the strong interaction with water molecules can simultaneously regulate the Zn2+ coordination environment facilitating the uniform deposition of Zn. As a consequence, only 0.5 wt% FI additive enables a highly reversible Zn plating/stripping over 4000 h at 1 mA cm−2, indicating a sufficient advance in performance over state‐of‐the‐art Zn anodes. Furthermore, when applied to a full battery (NaVO/Zn), the cell exhibits excellent capacity retention of 98.4% after 1000 cycles as well as high Coulombic efficiency of 99%, whereas the cell only operates for 68 cycles without FI additive. This work offers a non‐toxic, low‐cost, effective additive strategy to solve dendrites problems and achieve long‐life and high‐performance rechargeable aqueous ZIBs.

The kinetic mechanisms underlying the bottom-up assembly of colloidal particles have been widely investigated in efforts to control crystallization pathways and to direct growth into targeted superstructures for applications, including photonic crystals. Current work builds on recent progress in the development of kinetic theories for crystal growth of bcc crystals in systems with short-range interparticle interactions, accounting for a greater diversity of crystal structures (including fcc and noncubic crystals) and the role of the longer-ranged interactions and orientational degrees of freedom arising in polar systems. We address the importance of orientational ordering processes in influencing crystal growth in such polar systems, thus advancing the theory beyond the treatment of the translational ordering processes considered in previous investigations. The work employs comprehensive molecular dynamics simulations that resolve key crystallization processes and are used in the development of a quantitative theoretical framework based on ideas from time-dependent Ginzburg–Landau theory. The significant effect of orientational ordering (polarization or magnetization) on the crystallization kinetics could be potentially leveraged to achieve solidification kinetics steering through external electric or magnetic fields. Our combined theory/simulation approach provides opportunities for future investigations of more complex crystallization kinetics.

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