Operando Imaging-Guided Gradient Design for High-Mass-loading Cathodes

September 15, 2025
a) Position vs. time plots with the averaged neutron transmission (trans.) changes (Trt/Tr0) represented in color. Trt/Tr0<1 indicates reduced trans. due to Li increase or natLi replaced by 6Li, Trt/Tr0>1 indicates increased trans. due to delithiation. (b) Zoomed in on the cathode side. Colormap has been slightly changed to enhance the contrast for better visualization. Voltage vs. time curve is overlayed in white color.

Scientific Achievement

Directly visualized Li reaction gradients in thick, high-mass-loading all-solid-state batteries (ASSBs) cathodes. A Li⁺ flux–guided gradient catholyte design was developed, enabling superior rate capability.

Significance and Impact

This work provides the first direct evidence of Li⁺ flux mismatch in thick solid-state cathodes and offers a scalable design principle to overcome it. 

Research Details

A 33 mg/cm² NMC811 cathode was monitored using operando neutron imaging. Lithiation inhomogeneity from the solid electrolyte (SE) side to the current collector was observed. A three-layer cathode—graded in SE content from high to low—significantly improved rate performance for NMC811 and lithium cobalt oxide (LCO) cathodes, with up to 171% capacity gain at high current. 

 

Operando Neutron Imaging-Guided Gradient Design of Li-ion Solid Conductor for High-Mass-loading Cathodes,“ Nature Communications, 16 (7667) (2025)
https://doi.org/10.1038/s41467-025-62518-y