Abstract
We use in situ synchrotron X-ray diffraction measurements to monitor the solvothermal crystallisation mechanism of the aperiodic metal–organic framework TRUMOF-1. Following an initial incubation period, TRUMOF-1 forms as a metastable intermediate that subsequently transforms into an ordered product with triclinic crystal symmetry. We determine the structure of this ordered phase, which we call P1-TRUMOF-1, and show that it is related to TRUMOF-1 through topotactic reorganisation of linker occupancies. Our results imply that the degree and nature of correlated disorder in TRUMOF-1 is not fixed, and might be synthetically tuned as required for data storage and manipulation applications.