Metal–polyphenol networks (MPNs) are being used as versatile coatings for regulating membrane surface chemistry and for the formation of thin separation layers. The intrinsic nature of plant polyphenols and their coordination with transition metal ions provide a green synthesis procedure of thin films, which enhance membrane hydrophilicity and fouling resistance. MPNs have been used to fabricate tailorable coating layers for high-performance membranes desirable for a wide range of applications. Here, we present the recent progress of the use of MPNs in membrane materials and processes with a special focus on the important roles of tannic acid–metal ion (TA-Mⁿ⁺) coordination for thin film formation. This review introduces the most recent advances in the fabrication techniques and the application areas of TA-Mⁿ⁺ containing membranes. In addition, this paper outlines the latest research progress of the TA–metal ion containing membranes and summarizes the role of MPNs in membrane performance. The impact of fabrication parameters, as well as the stability of the synthesized films, is discussed. Finally, the remaining challenges that the field still faces and potential future opportunities are illustrated.

Thin-film composite (TFC) membranes containing a metal–polyphenol network (MPN)-based selective layer were fabricated on a porous polyacrylonitrile support. The MPN layer was formed through coordination-based self-assembly between plant-based tannic acid (TA) and an Fe³⁺ ion. For the first time, we demonstrate that TFC membranes containing TA-Fe³⁺ selective layers can separate small organic solutes in aqueous media from equimolar mixtures of solutes. The effect of the assembly time on the characteristics and performance of the fabricated selective layer was investigated. An increase in the assembly time led to the formation of selective layers with smaller effective pore sizes. The tannic acid–Fe³⁺ selective layer exhibited a low rejection towards neutral solutes riboflavin and poly(ethylene glycol) while high rejections were observed for anionic dyes of orange II and naphthol green B. Permeation selectivities in the range of 2–27 were achieved between neutral and charged dyes in both single- and mixed-solute experiments, indicating the significant role of Donnan exclusion and the charge-selective nature of the membranes. The rejection efficiency improved with an increasing assembly time. Overall, this study demonstrates that the assembly time is a vital casting parameter for controlling the permeance, rejection and selectivity of thin-film composite membranes with a tannic acid–Fe³⁺ selective layer.

Tannic acid (TA)–Fe³⁺ membranes have received recent attention due to their sustainable method of fabrication, high water flux and organic solutes rejection performance. In this paper, we present a description of the transport of aqueous solutions of dyes through these membranes using the transport parameters of the Spiegler–Kedem–Katchalsky (SKK) model. The reflection coefficient (σ) and solute permeability ($P_S$) of the considered TA–Fe³⁺ membranes were estimated from the non-linear model equations to predict the retention of solutes. The coefficients σ and $P_S$ depended on the porous medium and dye molecular size as well as the charge. The simulated rejections were in good agreement with the experimental findings. The model was further validated at low permeate fluxes as well as at various feed concentrations. Discrepancies between the observed and simulated data were observed at low fluxes and diluted feed solutions due to limitations of the SKK model. This work provides insights into the mass transport mechanism of dye solutions and allows the prediction of dye rejection by the TFC membranes containing a TA–Fe³⁺ selective layer using an SKK model.