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Using cryogenic transmission electron microscopy, we revealed three dimensional (3D) structural details of the electrochemically plated lithium (Li) flakes and their solid electrolyte interphase (SEI), including the composite SEI skin-layer and SEI fossil pieces buried inside the Li matrix. As the SEI skin-layer is largely comprised of nanocrystalline LiF and Li2O in amorphous polymeric matrix, when complete Li stripping occurs, the compromised SEI three-dimensional framework buckles, forming nanoscale bends and wrinkles. We showed that the flexibility and resilience of the SEI skin-layer plays a vital role in preserving an intact SEI 3D framework after Li stripping. The intact SEI network enables the nucleation and growth of the newly plated Li inside the previously formed SEI network in the subsequent cycles, preventing additional large amount of SEI formation between newly plated Li metal and the electrolyte. In addition, cells cycled under the accurately controlled uniaxial pressure can further enhance the repeated utilization of the SEI framework and improve the coulombic efficiency (CE) by up to 97%, demonstrating an effective strategy of reducing the formation of additional SEI and inactive dead Li. The identification of such flexible and porous 3D SEI framework clarifies the working mechanism of SEI in lithium metal anode for batteries. The insights provided in this work will inspire researchers to design more functional artificial 3D SEI on other metal anodes to improve rechargeable metal battery with long cycle life.
Crystallography, the primary method for determining the three-dimensional (3D) atomic positions in crystals, has been fundamental to the development of many fields of science. However, the atomic positions obtained from crystallography represent a gl
The solid electrolyte interphase (SEI) is regarded as the most complex but the least understood constituent in secondary batteries using liquid and solid electrolytes. The nanostructures of SEIs were recently reported to be equally important to the c
We develop in this paper a novel intrinsic classification algorithm -- multi-frequency class averaging (MFCA) -- for classifying noisy projection images obtained from three-dimensional cryo-electron microscopy (cryo-EM) by the similarity among their
The 3D ternary Li_4Ti_5O_12, the Li+-based battery anode, presents the unusual lattice symmetry (a triclinic crystal), band structure, charge density, and density of states, under the first-principles calculations. It belongs to a large direct-gap se
Next generation batteries based on lithium (Li) metal anodes have been plagued by the dendritic electrodeposition of Li metal on the anode during cycling, resulting in short circuit and capacity loss. Suppression of dendritic growth through the use o