Correlating Structure and Function of Battery Interphases at Atomic Resolution Using Cryoelectron Microscopy

Abstract

The solid electrolyte interphase (SEI) forms on all lithium battery anodes during operation and dictates their performance. Using cryoelectron microscopy, we stabilize these reactive materials for atomic-scale observation and correlate their nanostructure with battery performance. By imaging at various stages of battery operation, we reveal that the distribution of crystalline domains within the SEI is critical for the uniform transport of lithium ions. This establishes the important role that the SEI nanostructure plays in determining the performance of a battery.

A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions

“…LiF,L iN x O y ,a nd Li 2 Oa re mixed in spatial, forming abundant heterogeneous grain boundaries.T he grain boundaries between inorganics significantly impact the diffusion of Li ions in SEI. [15,55] There are much different grain boundaries in SEI, mainly including heterogeneous and homogeneous grain boundaries.T he heterogeneous grain boundaries are proven to exhibit the faster diffusion of Li ions than the homogeneous grain boundaries. [59] Thed iffusion of Li ions in SEI are positively correlated with exchange current density (I 0 ,F igure 3h).…”

“…Generally,t he formation of Li dendrites was induced by non-uniform SEI during the plating process in Li metal batteries. [12,13] Theg rowth of Li dendrites cracks fragile SEI during Li plating,a nd then induces side reactions between fresh Li and electrolyte, [14] i.e., SEI precursors.A fterwards during Li stripping process,p arts of the plated Li loses electronic contact with the current collectors forming dead Li due to uneven stripping rate, [15] which also causes the depletion of fresh Li. Moreover,t he depletion amount of fresh Li and electrolyte per cycle increase with the increasing cycling capacity,i .e., high loading cathode of practical conditions.T herefore,i ntrinsically uniform SEI is the footstone of the design principles of SEI under practical conditions to regulate Li deposition and mitigate the depletion of SEI precursors.…”

A compact inorganic layer for robust anode protection in lithium‐sulfur batteries

“…The corrosion of Li metal can be attributed to the following two reasons: (a) Li metal is highly reactive toward almost all nonaqueous solvents and Li salts in nature, generating solid electrolyte interphase (SEI) on the surface of Li anode . Moreover, dendritic Li forms and cracks the fragile SEI during Li plating . The rupture of SEI aggravates the side reactions between Li and electrolyte.…”

“…16 Moreover, dendritic Li forms and cracks the fragile SEI during Li plating. 17,18 The rupture of SEI aggravates the side reactions between Li and electrolyte. The nonstopping side reactions deteriorate the utilization efficiency of Li anode and cycling performance of batteries.…”

Li+‐Containing, Continuous Silica Nanofibers for High Li+ Conductivity in Composite Polymer Electrolyte

“…Conventional organic liquid electrolytes cooperating with highly reactive Li metal anodes, usually cause severe safety issues owing to the infinite dendritic Li growth, unstable solid‐electrolyte interphase formation, separators failure, and internal short circuits . The flammable liquid electrolytes further exacerbate the safety hazards and result in fires or even explosions .…”