Architecting highly hydratable and permeable dense Janus membrane for rapid and robust membrane distillation desalination

•High-performance dense JM was facily designed through a IP reaction utilzing THPC monomer.•Flux of THPC/PVDF JM even increased by 21.3 %, avoiding sacrifice of flux as conventional dense JMs.•THPC/PVDF JM showed simultaneously robust wetting/fouling/scaling resistance.•THPC polymer network uniquely improved water absorption, permeability and IW content.•Synergy between lower evaporation enthalpy and adequate water supply is key to improve flux. Dense Janus membranes (JMs) are potential candidates in hypersaline wastewater treatments for membrane distillation (MD). However, dense surface layers generally add obvious membrane mass transfer resistance, limiting its practical application. In this study, a novel dense JM was facilely developed by controlled interfacial polymerization utilizing a phosphonium functional monomer (THPC) on hydrophilic polyvinylidene fluoride (PVDF) substrate. MD desalination performance results showed that the optimized THPC/PVDF JM surprisingly achieved a flux even 21.3 % higher than that of its substrate and exhibited robust stability to surfactants, oil, and gypsum. Importantly, potential mechanism of remarkable flux enhancement of dense JMs was revealed. Raman and DSC analyses showed that THPC/PVDF JM with elevated intermediate water content had minimal enthalpy for water evaporation, thus facilitating water vaporization. Dynamic water contact angle measurements, advanced microstructural characterization by positron annihilation spectroscopy and water permeability experiments etc. showed that THPC/PVDF JM with high hydrophilicity and appropriately enlarged effective pore sizes provided strong water-absorption capacity and water permeability, contributing to rapid water replenishment. Both synergistically contributed to an incredible increase in membrane flux. Meanwhile, the dense surface layer, featured by its strong hydrophilicity and abundant hydroxyl groups, effectively prevented complex contaminants from intruding hydrophobic substrate and discouraged oil/gypsum adhesion, ensuring stable MD operation. This study shall provide useful insights and strategies to design high-flux dense JMs with minimal membrane failure propensity, highlighting its great potential for efficient hypersaline wastewater treatments. [Display omitted]