Alignment of Breathing Metal–Organic Framework Particles for Enhanced Water-Driven Actuation

[Image: see text] As the majority of known metal–organic frameworks (MOFs) possess anisotropic crystal lattices and thus anisotropic physicochemical properties, a pressing practical challenge in MOF research is the establishment of robust and simple processing methods to fully harness the anisotropic properties of the MOFs in various applications. We address this challenge by applying an E-field to precisely align MIL-88A microcrystals and generate MIL-88A@polymer films. Thereafter, we demonstrate the impact of MOF crystal alignment on the actuation properties of the films as a proof of concept. We investigate how different anisotropies of the MIL-88A@polymer films, specifically, crystal anisotropy, particle alignment, and film composition, can lead to the synergetic enhancement of the film actuation upon water exposure. Moreover, we explore how the directionality in application of the external stimuli (dry/humid air stream, water/air interface) affects the direction and the extent of the MIL-88A@polymer film movement. Apart from the superior water-driven actuation properties of the developed films, we demonstrate by dynamometer measurements the higher degree of mechanical work performed by the aligned MIL-88A@polymer films with the preserved anisotropies compared to the unaligned films. The insights provided by this work into anisotropic properties displayed by aligned MIL-88A@polymer films promise to translate crystal performance benefits measured in laboratories into real-world applications. We anticipate that our work is a starting point to utilize the full potential of anisotropic properties of MOFs.