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Synthesis and application of antimicrobial poly(vinyl alcohol) electrospun nanofibers for water filtration : 항미생물 폴리비닐 알코올계 전기방사 나노파이버 제조 및 수처리 여과 적용

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dc.contributor.advisor김성배-
dc.contributor.author박정안-
dc.date.accessioned2017-07-13T17:42:04Z-
dc.date.available2017-07-13T17:42:04Z-
dc.date.issued2015-08-
dc.identifier.other000000066706-
dc.identifier.urihttps://hdl.handle.net/10371/121057-
dc.description학위논문 (박사)-- 서울대학교 대학원 : 생태조경·지역시스템공학부(지역시스템공학전공), 2015. 8. 김성배.-
dc.description.abstractThis thesis deals with the fabrication, characterization, and evaluation antimicrobial and anti-biofouling activity of electrospun poly (vinyl alcohol) (PVA) nanofibers with quaternary ammonium compound (QAC) and PVA/poly acrylic acid (PAA) nanofibers with protease for applying in water filtration. BTEAC-PVA electrospun nanofibers was fabricated via co-electrospinning, and PVA/PAA-Cu(II) containing α-chymotrypsin was synthesized with soaking treatment after electrospinning. The synthesized nanofibers were characterized by various analytical techniques such as SEM, EDS, DSC, TGA, FTIR, and CFP.
BTEAC-PVA nanofibers containing 2.6% BTEAC were fabricated to test the antibacterial and antiviral activities. For the BTEAC-PVA nanofibers, the bacterial reduction ratio increased with increasing contact time, demonstrating that BTEAC-PVA nanofibers successfully inhibited the growth of bacteria. In addition, the antiviral tests against viruses (bacteriophages MS2 and PhiX174) showed that the BTEAC-PVA nanofibers inactivated both MS2 and PhiX174. BTEAC-PVA deposited on GF membrane (BTEAC-PVA/GF ENMs) for increasing mechanical strength. BTEAC-PVA/GF ENMs were also examined water stability, flux, pore size, leaching, and D.magna toxicity that they are good candidate for environmental friendly micro-filter as water filter. After 10 ml filtration, 4.88 LRV (E. coli) and 5.75 LRV (S. aureus) was achieved using BTEAC-PVA/GF ENMs. Finally, 2.26 LRV (E. coli) and 3.29 LRV (S. aureus) was obtained after 500 ml filtrate volume with BTEAC-PVA/GF ENMs. The antibacterial water filtration test for river water were also performed that 67 CFU/mL (Total coliforms) in river water was removed all by BTEAC-PVA/GF ENMs during the filtration test. For anti-biofouling activity, deposited BTEAC-PVA on PC membrane (BTEAC-PVA/PC ENMs) could enhance the flux due to protect from biofouling of PC membrane with microorganism (K. pneumonia) solutions. Anti-biofouling effect was due to contact-dependent killing of sessile cells rather than reduction in the number of planktonic cells through biofouling resistance test. Antimicrobial mechanism of BTEAC-PVA nanofibers is damaging bacterial membrane observed by fluorescence microscopy and field emission scanning electron microscopy (FESEM) images. BTEAC-PVA/PC ENMs generally showed retaining antimicrobial activity over 6 cycles in regeneration study with bacteria, and mixed bacteria strain solution.
PVA/PAA nanofibers were successfully coordinated/chelated with Cu(II), then immobilization of α-chymotrypsin. The α-chymotrypsin is a proteas that could inhibit 53.50% of P. aeruginosa and 35.53% of S. aureus biofilm formation and reduce 58.2 % of P. aeruginosa biofilm and 43.5% of S. aureus biofilm with a microtiter assay. The Cu(II) adsorption capacity of PVA/PAA nanofibers is 44.85 mg/g (initial Cu(II) concentration = 500 mg/L, reaction time = 24 h) then immobilized amount of α-chymotrypsin on PVA/PAA-Cu(II) nanofibers is 25.56 ± 2.72 mg/g. PVA/PAA-Cu(II) nanofibers containing α-chymotrypsin have a good performance of anti-biofouling by reducing sessile cells via degrade EPS, especially protein.
The functionalized PVA nanofibers were applied as a water filter, and showed antibacterial and anti-biofouling performance with various tests including contact test, dynamic test, dead-end filtration test, and incubation test. In addition, this dissertation provides the possibility of eco-friendly approaches for the preparation of PVA based nanofibers containing QAC and protease, and their potential applications in water filtration.
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dc.description.tableofcontentsABSTRACT i
CONTENTS iv
LIST OF TABLES ix
LIST OF FIGURES xi

Chapter 1 Introduction 1
1.1 Background 2
1.1.1 Electrospun nanofibers for water filtration 2
1.1.2 Anti-biofouling activity using antimicrobial ENMs 4
1.1.3 Quaternary ammonium compound as antimicrobial agent 5
1.1.4 Enzymes as anti-biofouling agent 6
1.1.5 Poly (vinyl alcohol) (PVA) polymer 8
1.2 Objective 10

Chapter 2 Literature Review 18
2.1 Electrospun condition of PVA nanofiber 19
2.2 QAC functionalized electrospun nanofibers for antimicrobial and anti-fouling activity in aqueous solution 22
2.3 Enzyme immobilized on electrospun nanofibers for anti-biofouling 23
2.4 Electrospun PVA nanofibers for water treatment 25

Chapter 3 Preparation and Characterization of Antimicrobial Electrospun Poly(vinyl alcohol) Nanofibers Containing Benzyl Triethylammonium chloride 31
3.1 Materials and methods 32
3.1.1 Electrospinning of PVA nanofibers 32
3.1.2 Electrospinning of BTEAC-PVA nanofibers 33
3.1.3 Characterization of PVA and BTEAC-PVA nanofibers 34
3.1.4 Antibacterial tests 35
3.1.5 Antiviral tests 37

3.2 Results and discussion 39
3.2.1 Electrospun PVA nanofibers 39
3.2.2 Electrospun BTEAC-PVA nanofibers 44
3.2.3 FT-IR, TGA and EDS analyses 50
3.2.4 Antibacterial tests 53
3.2.5 Antiviral tests 60

Chapter 4 Functionalization of Poly(vinyl alcohol) Electrospun Nanofibrous Membranes with Benzyl Triethylammonium Chloride for Antimicrobial Water Filtration 62
4.1 Materials and methods 63
4.1.1 Fabrication of ENMs 63
4.1.2 Characterization of ENMs 64
4.1.3 Immersion, leaching, and toxicity tests for BTEAC 66
4.1.4 Antimicrobial water filtration tests 67

4.2 Results and discussion 70
4.2.1 Characteristics of BTEAC-PVA ENMs 70
4.2.2 BTEAC leaching and toxicity 75
4.2.3 Antibacterial assessment with filtration test 82
4.2.4 Antiviral water filtration tests 89

Chapter 5 Anti-biofouling Activity of Poly(vinyl alcohol) Electrospun Nanofibrous Membranes with Benzyl Triethylammonium Chloride 92
5.1 Materials and methods 93
5.1.1 Electrospun BTEAC-PVA ENMs 93
5.1.2 Characterization of BTEAC-PVA ENMs 94
5.1.3 Anti-biofouling activity of BTEAC-PVA ENMs 95
5.1.3.1 Anti-fouling activity by contact killing 95
5.1.3.2 Anti-fouling activity by preventing biofilm formation 97

5.2 Results and discussion 98
5.2.1 Characteristics of BTEAC-PVA/PC ENMs 98
5.2.1.1 Morphology 98
5.2.1.2 Swelling property of BTEAC-PVA nanofibers 100
5.2.1.3 Water permeability evaluation 103
5.2.1.4 Retaining BTEAC from BTEAC-PVA nanofibers 107
5.2.2 Evaluation of BTEAC-PVA ENMs anti-biofouling 109
5.2.2.1 The effect of contact time for contact killing 109
5.2.2.2 The effect of the number of bacteria for contact killing 113
5.2.2.3 Regeneration studies for contact killing 118
5.2.2.4 Preventing biofilm formation 120

Chapter 6 Immobilization of α-Chymotrypsin on Electrospun Poly(vinyl alcohol) /Poly(acrylic acid) Nanofibers for Anti-biofouling Activity 122
6.1 Materials and methods 123
6.1.1 Microtiter assay for biofilm removal and preventing biofilm formation using enzymes 123
6.1.2 Electrospinning of PVA/PAA nanofibers 124
6.1.3 Preparation of PVA/PAA-Cu(II) nanofibers 125
6.1.4 Immobilization of protease on PVA/PAA-Cu(II) nanofibers 126
6.1.5 Characterization of PVA-PAA nanofibers 127
6.1.6 Degradation of biofilm EPS using PVA/PAA-Cu (II)-α nanofibers 128
6.1.7 Anti-biofouling activity of adhesion-inhibition 129

6.2 Results and discussion 130
6.2.1 Effect of enzyme treatment on formation and removal of biofilms 130
6.2.2 Electrospun PVA/PAA nanofibers 134
6.2.3 Preparation of PVA/PAA-Cu(II)-α nanofibers 137
6.2.4 Degradation of EPS from PVA/PAA-Cu(II)-α nanofibers 143
6.2.5 Anti-biofouling activity of PVA/PAA-Cu(II)-α nanofibers 147

Chapter 7 General Conclusions and Recommendations 149
7.1 General Conclusions 150
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dc.formatapplication/pdf-
dc.format.extent12042707 bytes-
dc.format.mediumapplication/pdf-
dc.language.isoen-
dc.publisher서울대학교 대학원-
dc.subject전기방사-
dc.subject폴리비닐 알코올계-
dc.subject항미생물-
dc.subject4차 암모늄 화합물-
dc.subject프로테아제-
dc.subject수처리 여과-
dc.subject.ddc712-
dc.titleSynthesis and application of antimicrobial poly(vinyl alcohol) electrospun nanofibers for water filtration-
dc.title.alternative항미생물 폴리비닐 알코올계 전기방사 나노파이버 제조 및 수처리 여과 적용-
dc.typeThesis-
dc.contributor.AlternativeAuthorPark Jeong-Ann-
dc.description.degreeDoctor-
dc.citation.pagesxiv, 188-
dc.contributor.affiliation농업생명과학대학 생태조경·지역시스템공학부-
dc.date.awarded2015-08-
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