Heterostructured Interface Enables Uniform Zinc Deposition for High-Performance Zinc-Ion Batteries.

Zinc metal has considerable potential as a high-energy anode material for aqueous batteries due to its high theoretical capacity and environmental friendliness. However, dendrite growth and parasitic reactions at the electrode/electrolyte interface remain two serious problems for the Zn metal anode. Here, the heterostructured interface of ZnO rod array and CuZn5 layer is fabricated on the Zn substrate (ZnCu@Zn) to address these two issues. The zincophilic CuZn5 layer with abundant nucleation sites ensures the initial uniform Zn nucleation process during cycling. Meanwhile, the ZnO rod array grown on the surface of the CuZn5 layer can guide the subsequent homogeneous Zn deposition via spatial confinement and electrostatic attraction effects, leading to the dendrite-free Zn electrodeposition process. Consequently, the derived ZnCu@Zn anode exhibits an ultra-long lifespan of up to 2500 h with symmetric cells at the current density and capacity of 0.5 mA cm-2 /0.5 mA h cm-2 . Besides, a remarkable cyclability (75% retention for 2500 cycles at 2 A g-1 ) is achieved in the ZnCu@Zn||MnO2 full cell with a capacity of 139.7 mA h g-1 . This heterostructured interface with specific functional layers provides a feasible strategy for the design of high-performance metal anodes.

Stable Li metal anode in a lithiophilic shuttle.

Suppressing severe lithium (Li) dendrite growth is a formidable challenge for high-energy-density lithium (Li) metal batteries (LMBs). Conventional lithiophilic coatings, despite their ability to improve the Li plating morphology, generate a compact conversion layer with a low electrolyte volume fraction, impeding the mass- and charge-transfers at the electrode interface and offsetting the benefits brought by lithiophilicity. Herein, a lithiophilic shuttle is obtained by the superposition of very thin layered copper oxide (L-CuO) flakes. After the conversion process, conjoined channels with a high electrolyte volume fraction can be maintained in the lithiophilic shuttle for fast and lateral Li+ transfer. In addition to the inherent high-Li-affinity and layered-structure-induced capacitive feature, the lithiophilic shuttle can afford stable and reversible Li plating/stripping at high current densities up to 3 mA cm-2 in LMBs with a practical capacity of 5 mA h cm-2. This work provides a new hierarchical lithiophilic structure to push forward high-energy-density LMBs for practical applications.

Theoretical description of molecular permeation via surface diffusion through graphene nanopores.

We establish a theoretical model to describe the surface molecular permeation through two-dimensional graphene nanopores based on the surface diffusion equation and Fick's law. The model is established by considering molecular adsorption and desorption from the surface adsorption layer and the molecular diffusion and concentration gradient on the graphene surface. By comparing with the surface flux obtained from molecular dynamics simulations, it is shown that the model can predict well the overall permeation flux especially for strongly adsorbed molecules (i.e. CO2 and H2S) on graphene surfaces. Although good agreement between the theoretical and simulated density distribution is hard to achieve owing to the large uncertainty in the calculation of surface diffusion coefficients based on the Einstein equation, the model itself is very competent to describe the surface molecular permeation both from the aspects of the overall permeation flux and detailed density distribution. This model is believed to supplement the theoretical description of molecular permeation through graphene nanopores and provide a good reference for the description of mass transport through two-dimensional porous materials.

Magnetohydrodynamic Interface-Rearranged Lithium Ions Distribution for Uniform Lithium Deposition and Stable Lithium Metal Anode.

Uneven lithium (Li) electrodeposition hinders the wide application of high-energy-density Li metal batteries (LMBs). Current efforts mainly focus on the side-reaction suppression between Li and electrolyte, neglecting the determinant factor of mass transport in affecting Li deposition. Herein, guided Li+ mass transport under the action of a local electric field near magnetic nanoparticles or structures at the Li metal interface, known as the magnetohydrodynamic (MHD) effect, are proposed to promote uniform Li deposition. The modified Li+ trajectories are revealed by COMSOL Multiphysics simulations, and verified by the compact and disc-like Li depositions on a model Fe3 O4 substrate. Furthermore, a patterned mesh with the magnetic Fe-Cr2 O3 core-shell skeleton is used as a facile and efficient protective structure for Li metal anodes, enabling Li metal batteries to achieve a Coulombic efficiency of 99.5 % over 300 cycles at a high cathode loading of 5.0 mAh cm-2 . The Li protection strategy based on the MHD interface design might open a new opportunity to develop high-energy-density LMBs.