Superwetting materials show great promise in emulsion separation. Herein, we developed superhydrophilic collagen fibers (CFs) by surface decoration of CFs with Zr4+, which were effective for dual separation of oil-in-water...

Developing high-performance separation membrane with good durability is a highly desired while challenging issue. Herein, we reported the successful fabrication of chemically and mechanically durable superhydrophobic membrane that was prepared by embedding UiO-66 as size-sieving sites within the supramolecular fiber structure of collagen fiber membrane (CFM), followed by the polydimethylsiloxane (PDMS) coating. The as-prepared CFM/UiO-66(12)/PDMS membrane featured capillary effect-enhanced separation flux and homogeneous porous channels guaranteed high separation efficiency. When utilized as double-layer separation membranes, this new type of composite membranes separated various surfactant stabilized water-in-oil microemulsions and nanoemulsions, with the separation efficiency high up to 99.993 % and the flux as high as 973.3 L m− 2 h− 1. Compared with commercial polytetrafluoro ethylene (PTFE) membrane, the advantage of the double-layer CFM/UiO-66(12)/PDMS membranes in separation flux was evident, which exhibited one order of magnitude higher than that of commercial PTFE membrane. The CFM/UiO-66(12)/PDMS membrane was acid-alkali tolerant, UV-aging resistant and reusable for emulsion separation. Notably, the CFM/UiO-66(12)/PDMS membrane was mechanically durable against strong mechanical abrasion, which was still capable of separating diverse water-in-oil emulsions after the abrasion with sandpaper and assembled as double-layer separation membranes. We anticipate that the combination of CFM and metal organic frameworks (MOFs) is an effective strategy for fabricating high-performance separation membrane with high mechanical and chemical durability. Graphical Abstract

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Separation plays a critical role in a broad range of industrial applications. Developing advanced separation materials is of great significance for the future development of separation technology. Collagen fibers (CFs), the typical structural proteins, exhibit unique structural hierarchy, amphiphilic wettability, and versatile chemical reactivity. These distinctive properties provide infinite possibilities for the rational design of advanced separation materials. During the past 2 decades, many progressive achievements in the development of CFs‐derived advanced separation materials have been witnessed already. Herein, the CFs‐based separation materials are focused on and the recent progresses in this topic are reviewed. CFs widely existing in animal skins display unique hierarchically fibrous structure, amphiphilicity‐enabled surface wetting behaviors, multi‐functionality guaranteed covalent/non‐covalent reaction versatility. These outstanding merits of CFs bring great opportunities for realizing rational design of a variety of advanced separation materials that were capable of achieving high‐performance separations to diverse specific targets, including oily pollutants, natural products, metal ions, anionic contaminants and proteins, etc. Besides, the important issues for the further development of CFs‐based advanced separation materials are also discussed.

Industrial manufacture generates a huge quantity of emulsion wastewater, which causes serious threats to the aquatic ecosystems. Water-in-oil (W/O) and oil-inwater (O/W) emulsions are two major types of emulsions discharged by industries. However, dual separation of W/O and O/W emulsions remains a challenging issue due to the contradictory permselectivity for separating the two emulsions. In the present investigation, the amphiphilicity-derived regional wetting mechanism of water and oil on the amphiphilic collagen fibers was revealed based on the combination of numerous experiments and molecular dynamics (MD) simulations. Electrostatic interactions and van der Waals force were manifested to be the driving forces of regional wetting in the hydrophilic and hydrophobic regions, respectively. The regional wetting endowed amphiphilic collagen fibers with underwater oleophobicity and underoil hydrophilicity, which enabled dual separation of emulsions by selectively retaining the dispersed water phase of W/O emulsions in the hydrophilic regions while the dispersed oil phase of O/W emulsions in the hydrophobic regions. The achieved separation efficiency was higher than 99.98%, and the flux reached 3337.6 L m −2 h −1 . Initial wetting status significantly affects the regional wetting-enabled dual separation. Based on the MD simulations, amphiphilic intramolecular conformations of tropocollagen were suggested to be the origins of regional wetting on collagen fibers. Our findings may pave the way for developing high-performance dual separation materials that are promising to be utilized for the practical treatment of emulsion wastewater.