Carbonate-based electrolytes in Li-ion batteries exhibit long range order in a frozen state, which enables their non-destructive analysis by diffraction methods. In the current study the spatial distribution of lithium and electrolyte inside the graphite anode was determined in cycled Li-ion cells using monochromatic spatially-resolved neutron diffraction measurements at 150 K. The results indicate a loss of lithium and electrolyte and their non-uniform distribution in the graphite anode in aged Li-ion cells. The observed lithium and electrolyte losses are directly correlated with two electrochemical performance degradation mechanisms, which are responsible for the cell capacity fade.

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The two‐dimensional lithium distribution in the graphite anode was non‐destructively probed by spatially resolved neutron diffraction for a batch consisting of 34 different cylinder‐type (18650) Li‐ion batteries in fully charged state. The uniformity of the lithium distribution was quantified and correlated to the cell specifications/electrochemistry and to intrinsic cell parameters like electrode thickness, position of current collectors, etc. which were obtained by X‐ray micro‐computed tomography. Non‐uniformities in the lithiation state of the anode from a constant plateau have been observed for the majority of the studied cells. Their location corresponds to the positions of current tabs connecting the electrode stripes and areas of incomplete electrode coating at the beginning and the end of the electrode stripes. Four commonly used schemes of current lid connection were identified. Each of them displays its own effect on the uniformity of the lithiation at the anode and, therefore, variation of the intrinsic state‐of‐charge distribution and, most probably, the ageing behavior of the electrodes.

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A series of low‐temperature studies on LiNi0.80Co0.15Al0.05O2 18650‐type batteries of high‐energy type with different stabilized states of fatigue is carried out using spatially resolved neutron powder diffraction, infrared/thermal imaging, and quasi‐adiabatic calorimetry. In‐plane distribution of lithium in the graphite anode and frozen electrolyte in fully charged state is determined non‐destructively with neutron diffraction and correlated to the introduced state of fatigue. An independent electrolyte characterization is performed via calorimetry studies on variously aged 18650‐type lithium‐ion batteries, where the shape of the thermodynamic signal is evolving with the state of fatigue of the cells. Analyzing the liquid electrolyte extracted/harvested from the studied cells reveals the decomposition of conducting salt to be the main driving factor for fatigue in the electrolyte degradation.

Lithium‐Ion Batteries In article number 2201652, Anatoliy Senyshyn and co‐workers investigate the degradation mechanisms of real life 18650‐type lithium‐ion batteries using a combination of neutron diffraction, calorimetry, infrared measurements, and chemical analytics of battery electrolytes. In addition to the increase of internal cell resistance, loss of movable lithium and “drying out” of the cell, they reveal decomposition of conducting salts to be the main driving factor in the electrolyte degradation.

The two-dimensional lithium distribution in the graphite anode was non-destructively probed by spatially resolved neutron diffraction for a batch consisting of 34 different cylinder-type (18650) Li-ion batteries in fully charged state. The uniformity of the lithium distribution was quantified and correlated to the cell specifications/electrochemistry and to intrinsic cell parameters like electrode thickness, position of current collectors, etc. which were obtained by X-ray micro-computed tomography. Non-uniformities in the lithiation state of the anode from a constant plateau have been observed for the majority of the studied cells. Their location corresponds to the positions of current tabs connecting the electrode stripes and areas of incomplete electrode coating at the beginning and the end of the electrode stripes. Four commonly used schemes of current lid connection were identified. Each of them displays its own effect on the uniformity of the lithiation at the anode and, therefore, variation of the intrinsic state-of-charge distribution and, most probably, the ageing behavior of the electrodes.

The Front Cover displays the lithium distribution in the graphite anode of 18650‐type Li−ion battery. A look into the cell's interior illustrates a non‐destructive character of the performed studies. The background template corresponds to the structure of lithiated graphite, referring to the diffraction technique as a tool for spatially resolved quantification of lithium concentration in the cell. More information can be found in the Article by A. Senyshyn and co‐workers.