In situ Synchrotron X‐ray Metrology Boosted by Automated Data Analysis for Real‐time Monitoring of Cathode Calcination

Synchrotron X-ray-based in situ metrology is advantageous for monitoring the synthesis of battery materials, offering high throughput, high spatial and temporal resolution, and chemical sensitivity. However, the rapid generation of massive data poses a challenge to on-site, on-the-fly analysis needed for real-time process monitoring. Here, a weighted lagged cross-correlation (WLCC) similarity approach is presented for automated data analysis, which merges with in situ synchrotron X-ray diffraction metrology to monitor the calcination process of the archetypal nickel-based cathode, LiNiO₂. The WLCC approach, incorporating variables that account for peak shifts and width changes associated with structural transformations, enables rapid extraction of phase progression within 10 seconds from tens of diffraction patterns. Details are captured, from initial precursors to intermediates and the final layered LiNiO₂, providing information for agile on-site adjustments during experiments and complementing post hoc diffraction analysis by offering insights into early-stage phase nucleation and growth. Expanding this data-powered platform paves the way for real time calcination process monitoring and control, which is pivotal to quality control in battery cathode manufacturing.