Water-Assisted Programmable Assembly of Flexible and Self-Standing Janus Membranes

Janus membranes with asymmetric wettability have been considered cutting-edge for energy/environmental-sustainable applications like water/fog harvester, breathable skin, and smart sensor; however, technical challenges in fabrication and accurate regulation of asymmetric wettability limit their development. Herein, by using water-assisted hydrogen-bonded (H-bonded) assembly of small molecules at water/oil interface, a facile strategy is proposed for one-step fabrication of membranes with well-regulable asymmetric wettability. Asymmetric orderly patterns, beneficial for mass transport based on abundant high-permeability sites and large surface area, are constructed on opposite membrane surfaces. Upon tuning water-assisted H-bonding via H-sites/configuration design and temperature/pH modulation, double-hydrophobic, double-hydrophilic, and hydrophobic-hydrophilic membranes are facilely fabricated. The Janus membranes show smart vapor-responsive curling and unidirectional water transport with promising flux of 1158±25 L m^-2  h^-1 under natural gravity and 31500±670 L·(m^-2  h^-1  bar^-1 ) at negative pressure. This bottom-up approach offers a feasible-to-scalable avenue to precise-manipulation of Janus membranes for advanced applications, providing an effective pathway for developing tailor-made self-assembled nanomaterials.