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Application of magnetic nanoparticles and reactive filter materials for wastewater treatment
KTH, School of Biotechnology (BIO), Industrial Biotechnology. (Bioprocess technology)
2013 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Lately sewage wastewater treatment processes (WWTP) are facing challenges due to strict regulations in quality of effluent standards and waste production. The reuse of wastewater treatment effluents is rapidly gaining attention as a means of achieving sustainable water supply. Therefore, new methods are required to achieve an efficient WWTP. The foremost emphasis of the present study is to investigate filter materials, synthesis, characterization, and application of magnetic nanoparticles (NPs) for WWTP. Primarily commercially available reactive filter materials such as Polonite and Sorbulite were tested for the effective reduction of contaminants in recirculation batch mode system. Secondly, the magnetic nanoparticles were synthesized using different techniques such as water-in-oil (w/o) microemulsion and co- precipitation methods and testing for their ability to remove contaminants from wastewater. Thirdly, toxicity test of magnetic NPs were performed using human keratinocytes (HaCaT) and endothelial (HMEC-1) cells (Papers I-VII).

The magnetic iron oxide nanoparticles (MION) synthesized using the co-precipitation method were further functionalized with tri-sodium citrate (TSC), 3-aminopropyl triethoxysilane (APTES), polyethylenimine (PEI) and chitosan. The functionalized MION were further characterized prior to use in removal of contaminants from wastewater. The sewage wastewater samples were collected from Hammarby Sjöstadsverk, Sweden and analyses were performed for the reduction of turbidity, color, total nitrogen, total organic carbon, phosphate and microbial content on the retrieval day.

The experimental results imply that Polonite and Sorbulite require high pH for the efficient reduction of phosphate and the reduction of microbes. Microemulsion prepared magnetic nanoparticles (ME-MION) showed ≈100% removal of phosphate in 20 minutes. Results from TEM implied that the size of magnetic Nps were around 8 nm for core (uncoated MION), TSC (11.5 nm), APTES (20 nm), PEI (11.8 nm) and chitosan (15 nm). Optimization studies using central composite face centered (CCF) design showed the potential of magnetic nanoparticles for the removal of turbidity (≈83%) and total nitrogen (≈33%) in 60 minutes. The sludge water content was reduced significantly by ≈87% when magnetic NPs were used whilst compared to the chemical precipitant used in WWTP. PEI coated MION showed ≈50% removal of total organic carbon from wastewater in 60 minutes. Effluents from wastewater treated with magnetic NPs were comparable with effluent from the present WWTP. There was no significant change observed in mineral ion concentration before and after treatment with MION. In addition, toxicity results from HMEC-1 and HaCaT cells revealed no formation of reactive oxygen species in the presence of magnetic NPs. Furthermore, laboratory experiments revealed the effectiveness and reusability of magnetic NPs. Thus magnetic NPs are a potential wastewater treatment agent and can be used for effective removal of contaminants, thereby reducing the process time, sludge water content and complex process steps involved in conventional WWTP.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2013. , ix, 63 p.
Series
TRITA-BIO-Report, ISSN 1654-2312 ; 2013:20
Keyword [en]
Reactive filter materials, magnetic nanoparticles, wastewater treatment process, nutrient reduction, sludge water content, toxicity of magnetic nanoparticles
National Category
Water Treatment Engineering and Technology Nano Technology
Identifiers
URN: urn:nbn:se:kth:diva-134236ISBN: 978-91-7501-948-2 (print)OAI: oai:DiVA.org:kth-134236DiVA: diva2:665773
Public defence
2013-12-12, FB54, Albanova Universitet Centrum, Roslagstullsbacken 21, Stockholm, 09:30 (English)
Opponent
Supervisors
Note

QC 20131121

Available from: 2013-11-21 Created: 2013-11-20 Last updated: 2014-03-13Bibliographically approved
List of papers
1. Efficacy of reactive mineral-based sorbents for phosphate, bacteria, nitrogen and TOC removal - Column experiment in recirculation batch mode
Open this publication in new window or tab >>Efficacy of reactive mineral-based sorbents for phosphate, bacteria, nitrogen and TOC removal - Column experiment in recirculation batch mode
2013 (English)In: Water Research, ISSN 0043-1354, E-ISSN 1879-2448, Vol. 47, no 14, 5165-5175 p.Article in journal (Refereed) Published
Abstract [en]

Two mineral-based materials (Polonite and Sorbulite) intended for filter wells in on-site wastewater treatment were compared in terms of removal of phosphate (PO4-P), total inorganic nitrogen (TIN), total organic carbon (TOC) and faecal indicator bacteria (Escherichia coli and Enterococci). Using an innovative, recirculating system, septic tank effluent was pumped at a hydraulic loading rate of 3000 L m(2) d(-1) into triplicate bench-scale columns of each material over a 90-day period. The results showed that Polonite performed better with respect to removal of PO4-P, retaining on average 80% compared with 75% in Sorbulite. This difference was attributed to higher CaO content in Polonite and its faster dissolution. Polonite also performed better in terms of removal of bacteria because of its higher pH value. The total average reduction in E. coli was 60% in Polonite and 45% in Sorbulite, while for Enterococci the corresponding value was 56% in Polonite and 34% in Sorbulite. Sorbulite removed TIN more effectively, with a removal rate of 23%, while Polonite removed 11% of TIN, as well as TOC. Organic matter (measured as TOC) was accumulated in the filter materials but was also released periodically. The results showed that Sorbulite could meet the demand in removing phosphate and nitrogen with reduced microbial release from the wastewater treatment process.

Keyword
Polonite, Sorbulite, Enterococci, Escherichia coli
National Category
Environmental Biotechnology Water Treatment
Identifiers
urn:nbn:se:kth:diva-131720 (URN)10.1016/j.watres.2013.05.056 (DOI)000324566400034 ()2-s2.0-84883285298 (Scopus ID)
Funder
Formas
Note

QC 20131018. Updated from "Manuscript" to "Article"

Available from: 2013-10-18 Created: 2013-10-17 Last updated: 2017-12-06Bibliographically approved
2. Microemulsion prepared magnetic nanoparticles for phosphate removal: Time efficient studies
Open this publication in new window or tab >>Microemulsion prepared magnetic nanoparticles for phosphate removal: Time efficient studies
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2014 (English)In: Journal of Environmental Chemical Engineering, ISSN 2213-3437, Vol. 2, no 1, 185-189 p.Article in journal (Refereed) Published
Abstract [en]

The present study investigates the effective removal of phosphate in sewage wastewater using magnetic iron oxide nanoparticles (MION). The microemulsion-prepared magnetic iron oxide nanoparticles (ME-MION) of around 7-10 nm was synthesized using water-in-oil microemulsion method. The interaction of ME-MION and phosphate was studied using In situ FT-IR technique. Batch experiments were carried out with wastewater to determine the conc. and time efficiency using ME-MION for removal of phosphate. The vibration peak at 1004 cm-1 and the presence of hydroxyl group (OH-) at 3673 cm-1 confirms the binding of phosphate to ME-MION. ME-MION with 0.44 g L-1 exhibited more than 95% phosphate reduction in 5 min and close to 100% in 20 min. Conversely the experimental data obtained has been fitted with Langmuir isotherm model and also exhibited high correlation coefficients. The ME-MION was regenerated and can be reused for minimum 5 consecutive times. Efficient and fast reduction of phosphate was attained while the recovery of nanoparticles was achieved by an external magnetic field. To the author's knowledge, this is the first report that underscores around 100% phosphate removal from wastewater using ME-MION in 20 min. The approach utilized in this study offers a potential technique in the reduction of phosphate in wastewater whilst, reducing the time and reuse of nanoparticles.

Keyword
FTIR, Magnetic nanoparticles, Microemulsion, Phosphate removal
National Category
Water Treatment Nano Technology
Identifiers
urn:nbn:se:kth:diva-134302 (URN)10.1016/j.jece.2013.12.008 (DOI)2-s2.0-84891814016 (Scopus ID)
Note

QC 20140203. Updated from submitted to published.

Available from: 2013-11-20 Created: 2013-11-20 Last updated: 2014-02-03Bibliographically approved
3. Effect of magnetic iron oxide nanoparticles in surface water treatment: Trace minerals and microbes
Open this publication in new window or tab >>Effect of magnetic iron oxide nanoparticles in surface water treatment: Trace minerals and microbes
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2013 (English)In: Bioresource Technology, ISSN 0960-8524, E-ISSN 1873-2976, Vol. 129, 612-615 p.Article in journal (Refereed) Published
Abstract [en]

The existing water treatment process often uses chemicals, which is of high health and environmental concern. The present study focused on the efficiency of microemulsion prepared magnetic iron oxide nanoparticles (ME-MIONs) and protein-functionalized nanoparticles (MOCP. +. ME-MIONs) in water treatment. Their influence on mineral ions and microorganisms present in the surface water from lake Brunnsviken and örlången, Sweden were investigated. Ion analysis of water samples before and after treatment with nanoparticles was performed. Microbial content was analyzed by colony forming units (CFU/ml). The results impart that ME-MIONs could reduce the water turbidity even in low turbid water samples. Reduction of microbial content (98%) was observed at 37 °C and more than 90% reduction was seen at RT and 30 °C when compared to untreated samples from lake örlången. The investigated surface water treatment method with ME-MIONs was not significantly affecting the mineral ion composition, which implies their potential complement in the existing treatment process.

Keyword
Lake water, Magnetic nanoparticles, Coagulant protein, Trace minerals, Microbes
National Category
Industrial Biotechnology
Identifiers
urn:nbn:se:kth:diva-127064 (URN)10.1016/j.biortech.2012.12.138 (DOI)000324566000083 ()2-s2.0-84873720387 (Scopus ID)
Note

QC 20130912

Available from: 2013-09-12 Created: 2013-08-28 Last updated: 2017-12-06Bibliographically approved
4. Application of Magnetic Nanoparticles for the removal of turbidity and total nitrogen from sewage wastewater: Modelling studies
Open this publication in new window or tab >>Application of Magnetic Nanoparticles for the removal of turbidity and total nitrogen from sewage wastewater: Modelling studies
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(English)Manuscript (preprint) (Other academic)
National Category
Water Treatment Nano Technology
Identifiers
urn:nbn:se:kth:diva-134303 (URN)
Note

QS 2013

Available from: 2013-11-20 Created: 2013-11-20 Last updated: 2015-11-17Bibliographically approved
5. Effective water content reduction in sewage wastewater sludge using magnetic nanoparticles
Open this publication in new window or tab >>Effective water content reduction in sewage wastewater sludge using magnetic nanoparticles
(English)Manuscript (preprint) (Other academic)
National Category
Water Treatment Nano Technology
Identifiers
urn:nbn:se:kth:diva-134304 (URN)
Note

QS 2013

Available from: 2013-11-20 Created: 2013-11-20 Last updated: 2013-11-21Bibliographically approved
6. Removal of total organic carbon from sewage wastewater using poly(ethylenimine)-functionalized magnetic nanoparticles
Open this publication in new window or tab >>Removal of total organic carbon from sewage wastewater using poly(ethylenimine)-functionalized magnetic nanoparticles
Show others...
2014 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 30, no 4, 1036-1044 p.Article in journal (Refereed) Published
Abstract [en]

The increased levels of organic carbon in sewage wastewater during recent years impose a great challenge to the existing wastewater treatment process (WWTP). Technological innovations are therefore sought that can reduce the release of organic carbon into lakes and seas. In the present study, magnetic nanoparticles (NPs) were synthesized, functionalized with poly(ethylenimine) (PEI), and characterized using TEM (transmission electron microscopy), X-ray diffraction (XRD), FTIR (Fourier transform infrared spectroscopy), CCS (confocal correlation spectroscopy), SICS (scattering interference correlation spectroscopy), magnetism studies, and thermogravimetric analysis (TGA). The removal of total organic carbon (TOC) and other contaminants using PEI-coated magnetic nanoparticles (PEI-NPs) was tested in wastewater obtained from the Hammarby Sjöstadsverk sewage plant, Sweden. The synthesized NPs were about 12 nm in diameter and showed a homogeneous particle size distribution in dispersion by TEM and CCS analyses, respectively. The magnetization curve reveals superparamagnetic behavior, and the NPs do not reach saturation because of surface anisotropy effects. A 50% reduction in TOC was obtained in 60 min when using 20 mg/L PEI-NPs in 0.5 L of wastewater. Along with TOC, other contaminants such as turbidity (89%), color (86%), total nitrogen (24%), and microbial content (90%) were also removed without significant changes in the mineral ion composition of wastewater. We conclude that the application of PEI-NPs has the potential to reduce the processing time, complexity, sludge production, and use of additional chemicals in the WWTP.

Keyword
Correlation spectroscopy, Magnetic nano-particles, Magnetization curves, Superparamagnetic behavior, Technological innovation, TEM (transmission electron microscopy), Total Organic Carbon, Wastewater treatment process
National Category
Water Treatment Nano Technology
Identifiers
urn:nbn:se:kth:diva-134305 (URN)10.1021/la404076n (DOI)000331015600010 ()2-s2.0-84893621759 (Scopus ID)
Funder
Science for Life Laboratory - a national resource center for high-throughput molecular bioscience
Note

QC 20140313. Updated from manuscript to article in journal.

Available from: 2013-11-20 Created: 2013-11-20 Last updated: 2017-12-06Bibliographically approved
7. Synthesis, characterization and toxicity assessment of magnetic nanoparticles on skin and endothelial cells in vitro: water treatment application
Open this publication in new window or tab >>Synthesis, characterization and toxicity assessment of magnetic nanoparticles on skin and endothelial cells in vitro: water treatment application
Show others...
(English)Manuscript (preprint) (Other academic)
National Category
Water Treatment Nano Technology Medical and Health Sciences
Identifiers
urn:nbn:se:kth:diva-134306 (URN)
Note

QS 2013

Available from: 2013-11-20 Created: 2013-11-20 Last updated: 2013-11-21Bibliographically approved

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