Suppressing electrolyte-lithium metal reactivity via Li+-desolvation in uniform nano-porous separator

Lithium reactivity with electrolytes leads to their continuous consumption and dendrite growth, which constitute major obstacles to harnessing the tremendous energy of lithium-metal anode in a reversible manner. Considerable attention has been focused on inhibiting dendrite via interface and electrolyte engineering, while admitting electrolyte-lithium metal reactivity as a thermodynamic inevitability. Here, we report the effective suppression of such reactivity through a nano-porous separator. Calculation assisted by diversified characterizations reveals that the separator partially desolvates Li+ in confinement created by its uniform nanopores, and deactivates solvents for electrochemical reduction before Li0-deposition occurs. The consequence of such deactivation is realizing dendrite-free lithium-metal electrode, which even retaining its metallic lustre after long-term cycling in both Li-symmetric cell and high-voltage Li-metal battery with LiNi0.6Mn0.2Co0.2O2 as cathode. The discovery that a nano-structured separator alters both bulk and interfacial behaviors of electrolytes points us toward a new direction to harness lithium-metal as the most promising anode.

Parallel-GPU-accelerated adaptive mesh refinement for three-dimensional phase-field simulation of dendritic growth during solidification of binary alloy

In the phase-field simulation of dendrite growth during the solidification of an alloy, the computational cost becomes extremely high when the diffusion length is significantly larger than the curvature radius of a dendrite tip. In such cases, the adaptive mesh refinement (AMR) method is effective for improving the computational performance. In this study, we perform a three-dimensional dendrite growth phase-field simulation in which AMR is implemented via parallel computing using multiple graphics processing units (GPUs), which provide high parallel computation performance. In the parallel GPU computation, we apply dynamic load balancing to parallel computing to equalize the computational cost per GPU. The accuracy of an AMR refinement condition is confirmed through the single-GPU computations of columnar dendrite growth during the directional solidification of a binary alloy. Next, we evaluate the efficiency of dynamic load balancing by performing multiple-GPU parallel computations for three different directional solidification simulations using a moving frame algorithm. Finally, weak scaling tests are performed to confirm the parallel efficiency of the developed code.

Zinc Anode for Mild Aqueous Zinc-Ion Batteries: Challenges, Strategies, and Perspectives

The rapid advance of mild aqueous zinc-ion batteries (ZIBs) is driving the development of the energy storage system market. But the thorny issues of Zn anodes, mainly including dendrite growth, hydrogen evolution, and corrosion, severely reduce the performance of ZIBs. To commercialize ZIBs, researchers must overcome formidable challenges. Research about mild aqueous ZIBs is still developing. Various technical and scientific obstacles to designing Zn anodes with high stripping efficiency and long cycling life have not been resolved. Moreover, the performance of Zn anodes is a complex scientific issue determined by various parameters, most of which are often ignored, failing to achieve the maximum performance of the cell. This review proposes a comprehensive overview of existing Zn anode issues and the corresponding strategies, frontiers, and development trends to deeply comprehend the essence and inner connection of degradation mechanism and performance. First, the formation mechanism of dendrite growth, hydrogen evolution, corrosion, and their influence on the anode are analyzed. Furthermore, various strategies for constructing stable Zn anodes are summarized and discussed in detail from multiple perspectives. These strategies are mainly divided into interface modification, structural anode, alloying anode, intercalation anode, liquid electrolyte, non-liquid electrolyte, separator design, and other strategies. Finally, research directions and prospects are put forward for Zn anodes. This contribution highlights the latest developments and provides new insights into the advanced Zn anode for future research.

Uniform Lithium Nucleation/Deposition Regulated by N/S Co-doped Carbon Nanospheres towards Ultra-stable Lithium Metal Anodes

Uncontrollable Li dendrite growth increases the risks of cell short-circuit or even safety accidents, severely hindering the practical application of lithium metal anodes (LMAs). Herein, the N/S-co-doped mesoporous carbon nanospheres...

Phase-field modeling of nonequilibrium solidification processes in additive manufacturing

This project models dendrite growth during nonequilibrium solidification of binary alloys using the phase-field method (PFM). Understanding the dendrite formation processes is important because the microstructural features directly influence mechanical properties of the produced parts. An improved understanding of dendrite formation may inform design protocols to achieve optimized process parameters for controlled microstructures and enhanced properties of materials. To this end, this work implements a phase-field model to simulate directional solidification of binary alloys. For applications involving strong nonequilibrium effects, a modified antitrapping current model is incorporated to help eject solute into the liquid phase based on experimentally calibrated, velocity-dependent partitioning coefficient. Investigated allow systems include SCN, Si-As, and Ni-Nb. The SCN alloy is chosen to verify the computational method, and the other two are selected for a parametric study due to their different diffusion properties. The modified antitrapping current model is compared with the classical model in terms of predicted dendrite profiles, tip undercooling, and tip velocity. Solidification parameters—the cooling rate and the strength of anisotropy—are studied to reveal their influences on dendrite growth. Computational results demonstrate effectiveness of the PFM and the modified antitrapping current model in simulating rapid solidification with strong nonequilibrium at the interface.

Multi-scale simulation of the dendrite growth during selective laser melting of rare earth magnesium alloy

The solidification microstructure of the alloy fabricated by the selective-laser-melting (SLM) process can significantly impact its mechanical properties. In this study, a multi-scale model which couples the macroscale model for thermal-fluid and microscale cellular automata (CA) was proposed to simulate the complex solidification evolution and the dendrite growth (from planar to cellular to dendritic growth) during the SLM process. The solid–liquid interface of CA was dispersed with the bilinear interpolation method. On that basis, the curvature was accurately determined, and the calculation result was well verified by employing the Kurz–Giovanola–Trivedi analytical solution. The dendrite morphology, solute distribution, and primary dendrite arm spacing during the solidification of the SLM molten pool were quantitatively analyzed with the proposed model, well consistent with the experiment. The distribution of the undercooling field and the concentration field at the tip of dendrites different orientations were analyzed, and the two competing growth mechanisms of converging and diverging growth were revealed. Moreover, the research also indicates that during the growth of dendrites, the result of dendrite competition is determined by the height of the dendrite tip position in the direction of the thermal gradient, while the distribution of the concentration field (symmetrical or asymmetric) at the tip of the dendrite critically impacted the competing growth form of dendrites.