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Role of membrane pore polymerization conditions for pH responsive behavior, catalytic metal nanoparticle synthesis, and PCB degradation

Producción científica: Articlerevisión exhaustiva

35 Citas (Scopus)

Resumen

This article describes the effects of changing monomer and cross-linker concentrations on the mass gain, water permeability, Pd-Fe nanoparticle (NP) loading, and the rate of degradation of 3,3’,4,4’,5-pentachlorobiphenyl (PCB 126) of pore functionalized polyvinylidene fluoride (PVDF) membranes. In this study, monomer (acrylic acid (AA)) and cross-linker (N, N′- methylene-bis (acrylamide)) concentrations were varied from 10 to 20 wt% of polymer solution and 0.5–2 mol% of monomer concentration, respectively. Results showed that responsive behavior of membrane could be tuned in terms of water permeability over a range of 270–1 L m−2 h−1 bar−1, which is a function of water pH. The NP size on the membrane surface was found in the range of 16–23 nm. With increasing cross-linker density the percentage of smaller NPs (< 10 nm) increases due to smaller mesh size formation during in-situ polymerization of membrane. NP loading was found to vary from 0.21 to 0.94 mg per cm2 of membrane area depending on the variation of available carboxyl groups in membrane pore domain. The NPs functionalized membranes were then tested for use as a platform for the degradation of PCB 126. The observed batch reaction rate (Kobs) for PCB 126 degradation for per mg of catalyst loading was found 0.08–0.1 h−1. Degradation study in convective flow mode shows 98.6% PCB 126 is degraded at a residence time of 46.2 s. The corresponding surface area normalized reaction rate (Ksa) is found about two times higher than Ksa of batch degradation; suggesting elimination of the effect of diffusion resistance for degradation of PCB 126 in convective flow mode operation. These Pd-Fe-PAA-PVDF membranes and nanoparticles are characterized by TGA, contact angle measurement, surface zeta potential, XRD, SEM, XPS, FIB, TEM and other techniques reveal the details about the membrane surface, pores and nanoparticles size, shape and size-distribution. Statistical analysis based on experimental results allows us to depict responsive behavior of functionalized membrane. In our best knowledge this paper first time reports detail study on responsive behavior of pore functionalized membrane in terms of permeability, NPs size, metal loading and its effect on PCB 126 degradation in a quantified approach.

Idioma originalEnglish
Páginas (desde-hasta)348-361
Número de páginas14
PublicaciónJournal of Membrane Science
Volumen555
DOI
EstadoPublished - jun 1 2018

Nota bibliográfica

Publisher Copyright:
© 2018 Elsevier B.V.

Financiación

This research is primarily supported by the NIH-NIEHS-SRC (Award number: P42ES007380 ). Partial support is also provided by NSF KY EPSCoR program (Grant number: 1355438 ). We thank John May and Megan Combs of Environmental Research and Training Laboratory (ERTL), University of Kentucky for GC-MS and ICP-OES analytical assistance. We also thank Dr. Dali Qian and Dr. Nicolas Briot of Electron Microscopy Center, University of Kentucky for extensive support to prepare samples for TEM and FIB instruments as well as to analyze TEM and FIB samples. Finally, we thank Matthew K. Defrese and Dr. Patrick J. Marsac, College of Pharmacy, University of Kentucky for helping us to conduct TG analysis in their laboratory. Appendix A

FinanciadoresNúmero del financiador
EPSCoR RID1355438
NIH-NIEHS-SRCP42ES007380
NSF

    ASJC Scopus subject areas

    • Biochemistry
    • General Materials Science
    • Physical and Theoretical Chemistry
    • Filtration and Separation

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