Mechanochemical Phase Engineering of Conductive Metal–Organic Frameworks

Crystallographic phase engineering plays a pivotal role in tailoring the physical and chemical properties of materials. In metal–organic frameworks (MOFs), phase transitions triggered by chemical or physical stimuli, which often involve high temperatures and pressures, have enabled structural modulation for applications in separation, catalysis, and energy storage. However, the mechanisms underlying these transformations are still unclear and the experimental conditions are often complicated and energy-consuming. Here, we propose a mechanochemical phase engineering (MPE) strategy that allows for the precise, low-energy control of phase transitions in conductive MOFs. We observed an interface-dominated in situ phase transformation in conductive MOFs, transitioning from a kinetically stable to a thermodynamically stable phase, and elucidated its underlying mechanism. This work not only provides fundamental insights into phase structure–function relationships but also establishes MPE as a scalable and sustainable route for designing multifunctional materials with tunable phase behavior, paving the way for the rational design of next-generation electronic and energy devices.