Haitang Zhang, Wenbin Tu, Xiaohong Wu, Jiyuan Xue, Yuan Tian, Jianken Chen, Qiongqiong Qi, Yeguo Zou, J. Wang, Jing‐Hua Tian, Yu Qiao, Shi‐Gang Sun
Despite considerable efforts devoted to the design and modification of advanced battery materials, lithium-ion batteries, especially those with high energy density, still face critical challenges such as safety risks and complex failure mechanisms. To tackle these issues, we developed a multimodal operando characterization platform for operating lithium-ion pouch cells. This platform combines several advanced operando diagnostic techniques, including infrared imaging, X-ray technologies, ultrasonic scanning, mass spectrometry, and gas chromatography-mass spectrometry. It allows nondestructively comprehensive and dynamic tracking of key operational parameters, such as temperature distribution, mechanical evolution, and gas evolution behavior. Moreover, we innovatively propose a concept of AI-driven closed-loop framework for battery operation, structured as "operando monitoring-data analysis-intelligent control", to efficiently process large amounts of data and deliver intelligent feedback. This work successfully achieves the real-time and nondestructive detection of various evolution behaviors during the operation of pouch lithium-ion batteries.