The composition, structure, and the formation mechanism of the solid–electrolyte interphase (SEI) in lithium-based (e.g., Li-ion and Li metal) batteries have been widely explored in the literature. However, very little is known about the ion transport through the SEI. Understanding the underlying ion diffusion processes across the SEI could lead to a significant progress, enabling the performance increase and improving safety aspects of batteries. Herein, we report the results of first-principles density functional theory calculations on the dominant diffusion pathways, energetics, and the corresponding diffusion coefficients associated with Li diffusion through the polycrystalline SEI. This paper is particularly concerned with the Li diffusion through the grain boundary (GB) formed between the three major inorganic components of the SEI, such as Li2O, LiF, and Li2CO3. It is found that Li diffusion occurs through the numerous open channels formed by the GB. The energetics and potential barriers vary significantly depending upon the structure of these channels, with the general trend being that Li diffusion in the GB is generally faster than in the neighboring crystalline regions within the grain interiors. In addition, the elastic properties of the GB are calculated allowing for more profound understanding of the SEI stability and formation.

Rechargeable zinc (Zn) batteries suffer from poor cycling performance that can be attributed to dendrite growth and surface-originated side reactions. Herein, we report that cycling performance of Zn metal anode can be improved significantly by utilizing monolayer graphene (Gr) as the electrodeposition substrate. Utilizing microscopy and X-ray diffraction techniques, we demonstrate that electrodeposited Zn on Gr substrate has a compact, uniform, and nondendritic character. The Gr layer, due to its high lattice compatibility with Zn, provides low nucleation overpotential sites for Zn electrodeposition. Atomistic calculations indicate that Gr has strong affinity to Zn (binding energy of 4.41 eV for Gr with four defect sites), leading to uniform distribution of Zinc adatoms all over the Gr surface. This synergistic compatibility between Gr and Zn promotes subsequent homogeneous and planar Zn deposits with low interfacial energy (0.212 J/m2) conformal with the current collector surface.

The temporal instability of a cylindrical capillary jet is analysed numerically for different liquid Reynolds numbers Re, disturbance wavenumbers k, and amplitudes ε0. The breakup mechanism of viscous liquid jets and the formation of satellite drops are described. The results show that the satellite size decreases with decreasing Re, and increasing k and ε0. Marginal Reynolds numbers below which no satellite drops are formed are obtained for a large range of wavenumbers. The growth rates of the disturbances are calculated and compared with those from the linear theory. These results match for low-Re jets, however as Re is increased the results from the linear theory slightly overpredict those from the nonlinear analysis. (At the wavenumber of k = 0.9, the linear theory underpredicts the nonlinear results.) The breakup time is shown to decrease exponentially with increasing the amplitude of the disturbance. The cut-off wavenumber is shown to be strongly dependent on the amplitude of the initial disturbance for amplitudes larger than approximately $\frac13$ of the initial jet radius. The stable oscillations of liquid jets are also investigated. The results indicate that liquid jets with Re ∼ O(1) do not oscillate, and the disturbances are overdamped. However, liquid jets with higher Re oscillate with a period which depends on Re and ε0. The period of the oscillation decreases with increasing Re at small ε0; however, it increases with increasing Re at large ε0. Marginal Reynolds numbers below which the disturbances are overdamped are obtained for a wide range of wavenumbers and ε0 = 0.05.

In the present work, taking advantage of aberration-corrected scanning transmission electron microscopy, we show that the dynamic lithiation process of anode materials can be revealed in an unprecedented resolution. Atomically resolved imaging of the lithiation process in SnO2 nanowires illustrated that the movement, reaction, and generation of b = [1[overline]1[overline]1] mixed dislocations leading the lithiated stripes effectively facilitated lithium-ion insertion into the crystalline interior. The geometric phase analysis and density functional theory simulations indicated that lithium ions initial preference to diffuse along the [001] direction in the {200} planes of SnO2 nanowires introduced the lattice expansion and such dislocation behaviors. At the later stages of lithiation, the Li-induced amorphization of rutile SnO2 and the formation of crystalline Sn and LixSn particles in the Li2O matrix were observed.

In lithium–oxygen batteries, the solubility of LiO2 intermediates in the electrolyte regulates the formation routes of the Li2O2 discharge product. High-donor-number electrolytes with a high solubility of LiO2 tend to promote the formation of Li2O2 large particles following the solution route, which eventually benefits the cell capacity and cycle life. Here, we propose that facet engineering of cathode catalysts could be another direction in tuning the formation routes of Li2O2. In this work, β-MnO2 crystals with high occupancies of {111} or {100} facets were adopted as cathode catalysts in Li–O2 batteries with a tetra­(ethylene)­glycol dimethyl ether electrolyte. The {111}-dominated β-MnO2 catalyzed the formation of the Li2O2 discharge product into large toroids following the solution routes, while {100}-dominated β-MnO2 facilitated the formation of Li2O2 thin films through the surface routes. Further computational studies indicate that the different formation routes of Li2O2 could be related to different adsorption energies of LiO2 on the two facets of β-MnO2. Our results demonstrate that facet engineering of cathode catalysts could be a new way to tune the formation route of Li2O2 in a low-donor-number electrolyte. We anticipate that this new finding would offer more choices for the design of lithium–oxygen batteries with high capacities and ultimately a long cycle life.