Order–Disorder\nTransition in Rutile VO<sub>2</sub>(M) Electrodes during Li Intercalation\nand Extraction

Transition metal oxides are widely employed as electrode\nmaterials\nin Li-ion batteries. During battery operation, Li ions are intercalated\nand extracted from the framework of the electrode structure, causing\nstructural transitions. In some materials, the process can drive order–disorder\ntransitions; however, insights into such processes are generally lacking,\nalthough they are essential for our understanding of battery aging\nand in the design of new sustainable battery chemistries. Herein,\nwe investigate the intercalation-induced order–disorder transition\nin rutile VO<sub>2</sub>(M) electrodes by means of galvanostatic charge/discharge\ncycling, <i>operando</i> powder X-ray diffraction, and total\nX-ray scattering with pair distribution function analysis. The study\nreveals that the rutile structure transforms irreversibly into a highly\ndisordered layered Li<sub><i>x</i></sub>VO<sub>2</sub> structure,\nwhich is capable of reversibly intercalating Li ions. Our findings\npoint out general trends for the intercalation-driven transitions\nin rutile oxides.