Pd/Fe nanoparticle integrated PMAA-PVDF membranes for chloro-organic remediation from synthetic and site groundwater

Hongyi Wan; Md Saiful Islam; Nicolas J. Briot; Matthew Schnobrich; Lucy Pacholik; Lindell Ormsbee; Dibakar Bhattacharyya

doi:10.1016/j.memsci.2019.117454

Pd/Fe nanoparticle integrated PMAA-PVDF membranes for chloro-organic remediation from synthetic and site groundwater

Hongyi Wan
, Md Saiful Islam
, Nicolas J. Briot
, Matthew Schnobrich
, Lucy Pacholik
, Lindell Ormsbee
, Dibakar Bhattacharyya

Research output: Contribution to journal › Article › peer-review

40 Scopus citations

Abstract

The poly(methacrylic acid) (PMAA) was synthesized in the pores of commercial microfiltration PVDF membranes to allow incorporation of catalytic palladium/iron (Pd/Fe) nanoparticles for groundwater remediation. Particles of 17.1 ± 4.9 nm size were observed throughout the pores of membranes using a focused ion beam. To understand the role of Pd fractions and particle compositions, 2-chlorobiphenyl was used as a model compound in solution phase studies. Results show H₂ production (Fe⁰ corrosion in water) is a function of Pd coverage on the Fe. Insufficient H₂ production caused by higher coverage (>10.4% for 5.5 wt%) hindered dechlorination rate. With 0.5 wt% Pd, palladized-Fe reaction rate (surface area normalized reaction rate, k_sa = 0.12 L/(m²-h) was considerably higher than isolated Pd and Fe particles. For groundwater, in a single pass of Pd/Fe-PMAA-PVDF membranes (0.5 wt% Pd), chlorinated organics, such as trichloroethylene (177 ppb) and carbon tetrachloride (35 ppb), were degraded to 16 and 0.3 ppb, respectively, at 2.2 seconds of residence time. The degradation rate (observed k_sa) followed the order of carbon tetrachloride > trichloroethylene > tetrachloroethylene > chloroform. A 36 h continuous flow study with organic mixture and the regeneration process show the potential for on-site remediation.

Original language	English
Article number	117454
Journal	Journal of Membrane Science
Volume	594
DOIs	https://doi.org/10.1016/j.memsci.2019.117454
State	Published - Jan 15 2020

Bibliographical note

Publisher Copyright:
© 2019 Elsevier B.V.

Funding

This work is supported by the NIEHS-SRP grant P42ES007380 . Partial support is also provided by NSF KY EPSCoR grant (Grant no: 1355438 ). We appreciate the suggestions and the work of Dr. Sebastián Hernández. We thank John May and Megan Combs from Environmental Research and Training Laboratory (ERTL) at UK for analytical assistance. We also appreciate the help provided by Paul Lee (Undergraduate Chemical Engineering Student) with some of the experiments on chlorinated organics. This work is supported by the NIEHS-SRP grant P42ES007380. Partial support is also provided by NSF KY EPSCoR grant (Grant no: 1355438). We appreciate the suggestions and the work of Dr. Sebastián Hernández. We thank John May and Megan Combs from Environmental Research and Training Laboratory (ERTL) at UK for analytical assistance. We also appreciate the help provided by Paul Lee (Undergraduate Chemical Engineering Student) with some of the experiments on chlorinated organics.

Funders	Funder number
Environmental Research and Training Laboratory (ERTL)
NIEHS-SRP	P42ES007380
National Science Foundation Arctic Social Science Program
Office of Experimental Program to Stimulate Competitive Research	1355438

Keywords

Chloro-organics removal
Focused ion beam
Groundwater remediation
H production
Pd/Fe membrane reactor

ASJC Scopus subject areas

Biochemistry
General Materials Science
Physical and Theoretical Chemistry
Filtration and Separation

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10.1016/j.memsci.2019.117454

Cite this

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title = "Pd/Fe nanoparticle integrated PMAA-PVDF membranes for chloro-organic remediation from synthetic and site groundwater",

abstract = "The poly(methacrylic acid) (PMAA) was synthesized in the pores of commercial microfiltration PVDF membranes to allow incorporation of catalytic palladium/iron (Pd/Fe) nanoparticles for groundwater remediation. Particles of 17.1 ± 4.9 nm size were observed throughout the pores of membranes using a focused ion beam. To understand the role of Pd fractions and particle compositions, 2-chlorobiphenyl was used as a model compound in solution phase studies. Results show H2 production (Fe0 corrosion in water) is a function of Pd coverage on the Fe. Insufficient H2 production caused by higher coverage (>10.4\% for 5.5 wt\%) hindered dechlorination rate. With 0.5 wt\% Pd, palladized-Fe reaction rate (surface area normalized reaction rate, ksa = 0.12 L/(m2-h) was considerably higher than isolated Pd and Fe particles. For groundwater, in a single pass of Pd/Fe-PMAA-PVDF membranes (0.5 wt\% Pd), chlorinated organics, such as trichloroethylene (177 ppb) and carbon tetrachloride (35 ppb), were degraded to 16 and 0.3 ppb, respectively, at 2.2 seconds of residence time. The degradation rate (observed ksa) followed the order of carbon tetrachloride > trichloroethylene > tetrachloroethylene > chloroform. A 36 h continuous flow study with organic mixture and the regeneration process show the potential for on-site remediation.",

keywords = "Chloro-organics removal, Focused ion beam, Groundwater remediation, H production, Pd/Fe membrane reactor",

author = "Hongyi Wan and Islam, \{Md Saiful\} and Briot, \{Nicolas J.\} and Matthew Schnobrich and Lucy Pacholik and Lindell Ormsbee and Dibakar Bhattacharyya",

note = "Publisher Copyright: {\textcopyright} 2019 Elsevier B.V.",

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doi = "10.1016/j.memsci.2019.117454",

language = "English",

volume = "594",

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AU - Wan, Hongyi

AU - Islam, Md Saiful

AU - Briot, Nicolas J.

AU - Schnobrich, Matthew

AU - Pacholik, Lucy

AU - Ormsbee, Lindell

AU - Bhattacharyya, Dibakar

PY - 2020/1/15

Y1 - 2020/1/15

N2 - The poly(methacrylic acid) (PMAA) was synthesized in the pores of commercial microfiltration PVDF membranes to allow incorporation of catalytic palladium/iron (Pd/Fe) nanoparticles for groundwater remediation. Particles of 17.1 ± 4.9 nm size were observed throughout the pores of membranes using a focused ion beam. To understand the role of Pd fractions and particle compositions, 2-chlorobiphenyl was used as a model compound in solution phase studies. Results show H2 production (Fe0 corrosion in water) is a function of Pd coverage on the Fe. Insufficient H2 production caused by higher coverage (>10.4% for 5.5 wt%) hindered dechlorination rate. With 0.5 wt% Pd, palladized-Fe reaction rate (surface area normalized reaction rate, ksa = 0.12 L/(m2-h) was considerably higher than isolated Pd and Fe particles. For groundwater, in a single pass of Pd/Fe-PMAA-PVDF membranes (0.5 wt% Pd), chlorinated organics, such as trichloroethylene (177 ppb) and carbon tetrachloride (35 ppb), were degraded to 16 and 0.3 ppb, respectively, at 2.2 seconds of residence time. The degradation rate (observed ksa) followed the order of carbon tetrachloride > trichloroethylene > tetrachloroethylene > chloroform. A 36 h continuous flow study with organic mixture and the regeneration process show the potential for on-site remediation.

AB - The poly(methacrylic acid) (PMAA) was synthesized in the pores of commercial microfiltration PVDF membranes to allow incorporation of catalytic palladium/iron (Pd/Fe) nanoparticles for groundwater remediation. Particles of 17.1 ± 4.9 nm size were observed throughout the pores of membranes using a focused ion beam. To understand the role of Pd fractions and particle compositions, 2-chlorobiphenyl was used as a model compound in solution phase studies. Results show H2 production (Fe0 corrosion in water) is a function of Pd coverage on the Fe. Insufficient H2 production caused by higher coverage (>10.4% for 5.5 wt%) hindered dechlorination rate. With 0.5 wt% Pd, palladized-Fe reaction rate (surface area normalized reaction rate, ksa = 0.12 L/(m2-h) was considerably higher than isolated Pd and Fe particles. For groundwater, in a single pass of Pd/Fe-PMAA-PVDF membranes (0.5 wt% Pd), chlorinated organics, such as trichloroethylene (177 ppb) and carbon tetrachloride (35 ppb), were degraded to 16 and 0.3 ppb, respectively, at 2.2 seconds of residence time. The degradation rate (observed ksa) followed the order of carbon tetrachloride > trichloroethylene > tetrachloroethylene > chloroform. A 36 h continuous flow study with organic mixture and the regeneration process show the potential for on-site remediation.

KW - Chloro-organics removal

KW - Focused ion beam

KW - Groundwater remediation

KW - H production

KW - Pd/Fe membrane reactor

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JO - Journal of Membrane Science

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M1 - 117454

ER -

Pd/Fe nanoparticle integrated PMAA-PVDF membranes for chloro-organic remediation from synthetic and site groundwater

Abstract

Bibliographical note

Funding

Keywords

ASJC Scopus subject areas

Access to Document

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