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Fabrication of Graphene and Molybdenum Disulfide Electrodes and Their Biosensor Applications : 그래핀과 이황화몰리브덴 전극의 제조 및 바이오센서로의 응용

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dc.contributor.advisor장정식-
dc.contributor.author안지현-
dc.date.accessioned2017-10-27T16:48:29Z-
dc.date.available2017-10-27T16:48:29Z-
dc.date.issued2017-08-
dc.identifier.other000000145464-
dc.identifier.urihttps://hdl.handle.net/10371/136879-
dc.description학위논문 (박사)-- 서울대학교 대학원 공과대학 화학생물공학부, 2017. 8. 장정식.-
dc.description.abstractBiosensors have received substantial attentions in analytical chemistry owing to their potential for a wide range of applications. Compared to various sensing methods, electrochemical sensing method is a very attractive and powerful tool for high-performance biosensors. Electrochemical biosensors recognize a measurable electrical signal through a transducer, leading to high sensitivity, low power consumption, simple instrumentation, and short analysis time. Among electrochemical biosensors, field-effect transistor (FET)-based sensors are promising candidates because of their ability to rapidly and sensitively detect analytes via efficient interfacial transfer of charge carriers. Transducers play a crucial role in improving the performance of FET sensors. From a material viewpoint, the characteristics of transducer materials significantly affect the sensing performance. Therefore, it is important to develop and utilize enhanced transducer materials for FET-type biosensors.
This dissertation describes CVD graphene and MoS2 as transducers for biosensor applications. Graphene, two-dimensinal (2D) structures with hexagonal lattice, comprises single- or few- layer of sp2-hybridized carbon atoms. Graphene has grabbed considerable focus owing to its outstanding thermal, mechanical, and electrical properties. Transition metal dichalcogenides (TMDs) are graphene-like 2D layered materials. Molybdenum disulfide (MoS2), which is a layered TMD, features high carrier mobility and low noise level. From these attractive properties, three different nanostructures based on graphene and MoS2 were used as transducers for biosensors. First, graphene was prepared via chemical vapor deposition (CVD) process. CVD graphene was applied to HBsAg and taste sensors. Second, the flower-like MoS2 nanospheres were fabricated using a simple hydrothermal method. After vapor deposition polymerization (VDP), carboxylated polypyrrole-coated nanospheres showed improved performance in As(III) sensor. Lastly, MoS2 nanosheets were grown on graphene surface by hydrothermal process. The nanocomposite was applied to a highly sensitive nonenzymatic sensor for H2O2 detection. These transducer materials can provide enhanced sensing performance with high sensitivity, good selectivity, and rapid response for various sensor applications.
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dc.description.tableofcontents1. Introduction 1
1.1 Background 1
1.1.1 Biosensors 1
1.1.1.1 Recognition elements 4
1.1.1.2 Electrochemical sensing method 5
1.1.2 Transducer materials 9
1.1.2.1 CVD graphene 9
1.1.2.2 Transition metal dichalcogenide 13
1.1.2.3 Conducting polymers 16
1.1.3 Biosensor applications 19
1.1.3.1 Hepatitis B virus sensor 19
1.1.3.2 Taste sensor 20
1.1.3.3 Arsenic sensor 21
1.1.3.4 H2O2 sensor 23
1.2 Objectives and Outlines 25
1.2.1 Objectives 25
1.2.2 Outlines 25


2. Experimental Details 28
2.1 Fabrication of flexible graphene aptasensor for hepatitis B virus detection 28
2.1.1 Fabrication of CVD graphene 28
2.1.2 Fabrication of hepatitis B sensor based on binding aptamer-conjugated graphene electrodes 29
2.1.3 Preparation of saliva sample 30
2.1.4 Characterization of hepatitis B sensor based on binding aptamer-conjugated graphene electrodes 30
2.1.5 Instruments for the hepatitis B sensor 31
2.2 Fabrication of duplex bioelectronic tongue based on multiplexed graphene electrodes for sensing umami and sweet tastes 32
2.2.1 Fabrication of CVD graphene on SiO2 wafer substrate 32
2.2.2 Fabrication of duplex graphene electrodes 33
2.2.3 Immobilization of nanovesicles on the DGE surface 34
2.2.4 Preparation of target tastants 34
2.2.5 Characterization of duplex bioelectronic tongue based on multiplexed graphene electrodes 35
2.2.6 Sensing measurements for the umami and sweet taste sensor 36
2.3 Fabrication of highly sensitive FET-type aptasensor using flower-like MoS2 nanospheres for real-time detection of arsenic(III) 37
2.3.1 Materials 37
2.3.2 Fabrication of flower-like MoS2 nanospheres 37
2.3.3 Fabrication of carboxylated polypyrrole-coated FMNSs 38
2.3.4 Fabrication of FET-type aptasensor for As(III) detection 39
2.3.5 Instrumentation for the FET-type aptasensor 39
2.3.6 Sensing measurements for the As(III) aptasensor 40
2.4 Fabrication of H2O2 sensor based on MoS2 nanosheets grown on CVD graphene 41
2.4.1 Materials 41
2.4.2 Preparation of CVD graphene 41
2.4.3 Fabrication of MoS2 nanosheets grown on the graphene substrate 42
2.4.4 Characterization of MoS2 nanosheets grown on the graphene substrate 43
2.4.5 Instruments for the H2O2 sensor 44

3. Results and Disccusions 45
3.1 Fabrication of flexible graphene aptasensor for hepatitis B virus detection 45
3.1.1 Fabrication of graphene based-aptasensor for hepatitis B virus detection 45
3.1.2 Characterization of flexible CVD graphene electrodes 49
3.1.3 Characterization of aptamer-immobilized graphene electrodes 53
3.1.4 Electrical properties of FET-type hepatitis B aptasensor 56
3.1.5 Real-time responses of FET aptasensor toward HBsAg 60
3.1.6 Real-time responses of FET aptasensor toward real samples 66
3.2 Fabrication of duplex bioelectronic tongue based on multiplexed graphene electrodes for sensing umami and sweet tastes 70
3.2.1 Fabrication of duplex bioelectronic tongue 70
3.2.2 Characterization of duplex bioelectronic tongue 74
3.2.3 Electrical properties of duplex bioelectronic tongue 81
3.2.4 Real-time responses of the DBT for umami tastant 84
3.2.5 Real-time responses of the DBT for umami tastant in artificial seasonings 89
3.2.6 Real-time responses of the DBT for sweet tastant 91
3.2.7 Dual responses of the DBT for umami and sweet tastants 95
3.3 Fabrication of highly sensitive FET-type aptasensor using flower-like MoS2 nanospheres for real-time detection of arsenic(III) 99
3.3.1 Fabrication of carboxylated polypyrrole-coated FMNSs 99
3.3.2 Characterization of FMNSs 106
3.3.3 Characterization of CFMNSs 112
3.3.4 Immobilization of aptamers on CFMNS surfaces 117
3.3.5 Electrical characteristics of CFMNSs 121
3.3.6 Real-time responses of CFMNS aptasensor toward arsenite 125
3.3.7 Real-time response of MoS2 based-aptasensor toward a real sample 131
3.4 Fabrication of H2O2 sensor based on MoS2 nanosheets grown on CVD graphene 135
3.4.1 Fabrication of MoS2 nanosheets grown on graphene substrate 135
3.4.2 Characterization of MNSCG 139
3.4.3 Electrical properties of MNSCG 146
3.4.4 Real-time responses of FET-type H2O2 biosensor based on MNSCG electrode 149
3.4.5 Selective response and reusability of MNSCG sensor 154
4. Conclusion 158
Reference 164
국문초록 177
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dc.formatapplication/pdf-
dc.format.extent5115188 bytes-
dc.format.mediumapplication/pdf-
dc.language.isoen-
dc.publisher서울대학교 대학원-
dc.subjectGraphene-
dc.subjectMolybdenum disulfide-
dc.subjectField-effect-transistor-
dc.subjectBiosensor-
dc.subject.ddc660.6-
dc.titleFabrication of Graphene and Molybdenum Disulfide Electrodes and Their Biosensor Applications-
dc.title.alternative그래핀과 이황화몰리브덴 전극의 제조 및 바이오센서로의 응용-
dc.typeThesis-
dc.description.degreeDoctor-
dc.contributor.affiliation공과대학 화학생물공학부-
dc.date.awarded2017-08-
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