Scalable fabrication of superhydrophilic membranes via polyphenol-driven sequential assembly engineering: Intensified hydration and robust crude oil fouling resistance

Despite decades of research, fabricating scalable biomimetic superhydrophilic membranes with robust crude oil repellency remains an unresolved industrial challenge, with critical unmet need. Here, we pioneer a polyphenol-driven sequential assembly strategy that constructs dual hydration barriers via iron-coordinated phytic acid (PA) immobilization on poly(vinyl alcohol)-tannic acid hydrogel-modified microfiltration substrates. This architecture achieves: (i) Unprecedented anti-crude oil adhesion through synergistic hydration layers, reducing flux decline to 10 % (vs. 23 % for co-assembled controls) during 1 h dead-end emulsion filtration; (ii) Enhanced mechanical robustness with 81.9 % and 59 % improvements in Young's modulus and tensile strength, respectively; (iii) Universal separation efficacy (>99 % for all oil-in-water emulsions) sustaining 747.3 L m⁻² h⁻¹ bar⁻¹permeance after 1 h cross-flow crude oil emulsion challenge; (iv) Scalable manufacturing under ambient conditions with <7 % property deviation across 0.112 m² specimens. The synergistic hydration barrier mechanism effectively suppresses viscous crude oil adhesion and fouling layer formation. This paradigm establishes a scalable platform for industrial antifouling membranes, demonstrating unprecedented consistency between nanoscale design and macroscale performance.