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Membranes containing reactive nanoparticles (Fe and Fe/Pd) immobilized in a polymer film (polyacrylic acid, PAA-coated polyvinylidene fluoride, PVDF membrane) are prepared by a new method. In the present work a biodegradable, non-toxic -“green” reducing agent, green tea extract was used for nanoparticle (NP) synthesis, instead of the well-known sodium borohydride. Green tea extract contains a number of polyphenols that can act as both chelating/reducing and capping agents for the nanoparticles. Therefore, the particles are protected from oxidation and aggregation, which increases their stability and longevity. The membrane supported NPs were successfully used for the degradation of a common and highly important pollutant, trichloroethylene (TCE). The rate of TCE degradation was found to increase linearly with the amount of Fe immobilized on the membrane, the surface normalized rate constant (kSA) being 0.005 L/m2h. The addition of a second catalytic metal, Pd, to form bimetallic Fe/Pd increased the kSA value to 0.008 L/m2h. For comparison purposes, Fe and Fe/Pd nanoparticles were synthesized in membranes using sodium borohydride as a reducing agent. Although the initial kSA values for this case (for Fe) are one order of magnitude higher than the tea extract synthesized NPs, the rapid oxidation reduced their reactivity to less than 20 % within 4 cycles. For the green tea extract NPs, the initial reactivity in the membrane domain was preserved even after 3 months of repeated use. The reactivity of TCE was verified with “real” water system.

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Functionalized membranes represent a field with multiple applications. Examination of specific metal−macromolecule interactions on these surfaces presents an excellent method for characterization of these materials. These interactions may also be exploited for heavy metal sorption from drinking and industrial water sources. Various low-capacity, silica-based ion-exchange and chelating sorbents (about 0.5 mmol of metal/g of resin) are available for treatment of such waters. Cellulosic membrane-based sorbents, functionalized with polyamino acids, present an excellent approach for high-capacity (3−14 mmol of metal/g of sorbent) metal sorption. Silica-based membrane sorbents possess metal sorption capacities approaching those of cellulosic-based membranes, with the added benefits of excellent acid and solvent resistance. Metal sorption capacities of silica-based membrane sorbents with various polyamino acids range from 0.6 mmol to 1.4 mmol of metal/g of sorbent. Ion exchange, chelation, and electrostatic interactions form the basis of metal sorption. Electrostatic interactions are greatly magnified in membrane-based sorbents, and are partly responsible for their high capacities. Regeneration of these sorbents has also been shown, including the possibility for selective desorption of metals.

Polycysteine and other polyamino acid functionalized microfiltration membrane sorbents work exceptionally well for the removal and recovery of toxic heavy metals from aqueous streams. These are high capacity sorbents (0.3-3.7 mg/cm2) with excellent accessibility and selectivity for heavy metals, such as Hg(II), Pb(II), and Cd(II) over nontoxic components such as calcium. Polycysteine functionalized membranes work particularly well for metals such as Hg(II) and Cd(II), even in high total dissolved solids containing streams. Parameters such as permeate flow rate,feed metal concentration, and counterion (for Hg(II)) have also been found to influence sorbent behavior. For multicomponent systems, polyglutamic acid functionalized membranes have been found to selectively sorb Pb(II) versus Cd(II). Selective sorption of Cr(III) has also been observed with actual waste streams containing several heavy metals, hardness, and high sodium (2,000 mg/L). The high capacity, site accessibility, and ease of regeneration of these membrane-based sorbents make them ideal for environmental separations when volume reduction or selective recovery is required.

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