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The use of natural compounds for preparing hybrid molecular films—such as surface coatings made from metal–phenolic networks (MPNs)—is of interest in areas ranging from catalysis and separations to biomedicine. However, to date, the film growth of MPNs has been observed to proceed in discrete steps (≈10 nm per step) where the coordination‐driven interfacial assembly ceases beyond a finite time (≈1...
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