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研究生(外文):Chou, Hung-Tao
論文名稱(外文):Syntheses of graphene-based materials for bioelectrochemical and photothermal applications
指導教授(外文):Tai, Nyan-Hwa
口試委員(外文):Lee, Chi-YoungLin, Jaeen-HorngChanh, Hwan-YouKuo, Wen-ShyongChen, Ying-Chieh
外文關鍵詞:graphenegraphene oxidemicrobial fuel cellbiosensorsmart glassfog harvestingphotothermal effect
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首先,本研究採用成本低廉、製程簡單之浸鍍方式製備碳材料浸鍍三聚氰胺海綿,以此作為微生物電池的陽極,提供一具備高生物相容性、利於大腸桿菌生長的導電網路。該結構具備多孔和高比表面積的特性,除了大幅提高大腸桿菌的貼覆面積外,亦具備良好的物質傳輸速率,顯著地提升微生物電池的表現,除了有極佳的電流密度輸出(可達335 A m-3)更大幅提升電池的耐久度,於37度環境下,電池可穩定運作20天。
接著本研究運用石墨烯高比表面積、高導電性和表面官能基眾多的特性,設計一結合鍍銀氧化石墨烯、铷錯合物和anti-T3抗體的奈米碳針,運用在電冷光奈米探針式生物傳感器中。該探針可藉由施以電力,電泳至陽極生成冷光,並藉此光學訊號判斷檢測物甲狀腺分子的濃度。結果顯示,其有效偵測區間為0.1 pg/mL到 0.8 ng/mL,偵測靈敏度可達0.05 pg/mL。此外,此奈米探針式生物傳感器在擬血漿的環境中運作依然具備良好的專一性
最後本研究以多巴胺為中間層、開發環保無毒、步驟簡易的碳纖維布改植方式,將二氧化鈦顆粒和PNIPAM分別嫁接於碳纖維布上,使其分別帶有超疏水和溫度響應的特性。藉由組合具備超疏水特性和親水特性兩種不同表面潤濕性的碳纖維布,於霧氣收集實驗中,可獲得206 mg cm-2h-1的收集效率。此外研究結果顯示,具備溫度響應特性的改質碳纖維布,在水氣逸散調節和紅外光雷射控制的液體閘道有極大的潛力。
This dissertation aims to explore bioelectrochemical- and photothermal-related applications using graphene-based composite materials. A highly durable microbial fuel cell (MFC) and a highly sensitive electrochemiluminescence (ECL) biosensor for the detection of 3,3′,5-triiodothyronine (T3) were designed using reduced graphene oxide as the coating material as well as the biomolecule carrier, attributing to high electroconductivity and high surface to volume ratio of graphene. In addition, because of the intrinsic high photothermal conversion rates, carbon materials integrated with poly(N- isopropylacrylamide) (PNIPAM) can be used for the applications of a smart window and a near-infrared (NIR) light-controllable valve.
First, through a facile and cost-effective dip-coating process, carbon materials-coated melamine sponge was fabricated for MFC’s bioanode, providing a conductive network for the transfer of electrons and excellent biocompatibility for the proliferation of Escherichia coli. The scaffold with high porosity and large specific area not only provided a large specific area for the immobilization of E. coli but also possessed high mass transfer rate, improving the MFC performance with a maximum current density of 335 Am3 and a remarkably durable lifetime of 20 days at 37 °C.
Then, a nanoprobe used in an ECL biosensor was designed, comprising three components, silver nanoparticles decorated with functionalized GO, a ruthenium complex, and an anti-T3 antibody, using the features of high aspect surface ratio, high conductivity, and numerous moieties of GO. By supplying electricity, the GO-based nanoprobe underwent electrophoresis to the anode at which ECL was induced, generating a signal corresponding to the T3 molecule concentration. T3 was quantitatively measured in the range from 0.1 pg/mL to 0.8 ng/mL with a detection limit of 0.05 pg/mL. In addition, the novel immunosensor exhibited good specificity in the presence of serum.
Subsequently, smart glasses loaded with GO-impregnated PNIPAM hydrogel were also prepared. By uniformly intercalating photothermic GO within a thermotropic PNIPAM hydrogel, this automatically smart glass could transform its transparency from 92% to 0% under the sunshine; as a result, screening sunlight and preventing further increase in temperature of a space. In addition, the GO-impregnated thermotropic hydrogel absorbed colored organic solvents, affording a smart glass with arbitrary color.
Finally, an eco-friendly, facile, and efficient method was proposed using dopamine as the base for the secondary immobilization of titanium oxide (TiO2) and PNIPAM on carbon fiber clothes (CFCs), which render CFCs with properties of superhydrophobicity and thermo-responsiveness. A CFC with periodic superhydrophobic-hydrophilic patterns comprising TiO2@CFC and PD-coated hydrophilic striped patterns exhibited excellent performance for water harvesting at rates of 206 mg cm2 h1. In addition, the results reported in the dissertation indicated that the modification of a surface with characteristics of temperature responsiveness demonstrates significant potential for the adjustment of water evaporation, as well as NIR-controllable valves.
摘要 II
Abstract III
誌謝 IV
Outline V
Table List VII
Figure List VIII
Chapter 1 Overview 1
1.1 Introduction to carbon materials 1
1.1.1 Graphene-based materials 2
1.1.2 Carbon nanotube/carbon fiber 3
1.1.3 Bioelectrochemical applications of graphene-based materials 5
1.1.4 Photothermal-related applications of graphene-based materials 7
1.2 Introduction to MFCs 8
1.2.1 Mechanism and category of MFCs 9
1.2.2 Applications of carbon materials in MFC 10
1.3 Introduction to electrochemiluminescence biosensors 12
1.3.1 Mechanism and category of ECL biosensors 12
1.3.2 Applications of carbon materials in ECL biosensors 14
1.4 Introduction to poly(N-isopropylacrylamide) (PNIPAM) 16
1.4.1 Grafting of PNIPAM 17
1.4.2 Applications of PNIAPM 18
1.4.3 Applications of carbon materials–PNIPAM hybrid composite 20
1.5 Aims of this investigation 22
1.6 Organization 22
Chapter 2 Experiments and Characterizations 36
2.1 Syntheses of graphene based materials 36
2.1.1 Synthesis of GO 36
2.1.2 Synthesis of functionalized GO (fGO) 37
2.1.3 Synthesis of RGO 37
2.1.4 Synthesis of functionalized RGO (fRGO) 38
2.1.5 Synthesis of functionalized MWCNT (fMWCNT) 38
2.2 Fabrications of composites 39
2.2.1 Preparation of sponges coated with fRGO and fMWCNT used as anode in MFC 39
2.2.2 Preparation of silver nanoparticle decorated fGO (Ag@fGO) and Ag@fGO-based nanoprobe used in biosensor 40
2.2.3 Preparation of PNIPAM hydrogel impregnated with GO (GO/PNIPAM) 41
2.2.4 Preparation of surface modified CFCs with TiO2 decoration or PNIPAM immobilization 41
2.3 Characterization technique 43
Chapter 3 Highly durable anodes of MFC using a reduced graphene oxide/carbon nanotube-coated scaffold 45
3.1 Research background 45
3.2 Experiments 45
3.3 Results and discussion 46
3.3.1 Characterization of carbon material 46
3.3.2 Morphologies of RGO/CNT sponge anode 48
3.3.3 Current output and durability of MFC 49
3.3.4 Quantity evaluation of bacteria colonised on anode 51
3.4 Summaries 53
Chapter 4 An ultrasensitive sandwich type electrochemiluminescence immunosensor for T3 detection using silver nanoparticle-decorated graphene oxide as a nanocarrier 63
4.1 Research background 63
4.2 Experiments 64
4.3 Results and discussion 65
4.3.1 Acting mechanism of the Ag@fGO-T3 ECL immunosensor 65
4.3.2 Characterization of Ag@fGO and Ag@fGO-T3 nanoprobe 66
4.3.3 ECL behavior of the immunosensors 68
4.3.4 Long-term performance, specificity and reproducibility of the immunosensor 70
4.4 Summaries 71
Chapter 5 Switchable transparency of dual-controlled smart glass prepared with hydrogel-containing graphene oxide for energy efficiency 84
5.1 Research background 84
5.2 Experiments 85
5.3 Results and discussion 86
5.3.1 Characterization of GO/PNIPAM 86
5.3.2 Optical characteristics of smart glass 88
5.3.3 Cooling capability of the hydrogel glass 90
5.3.4 Fabrication of colored smart glass 93
5.4 Summaries 94
Chapter 6 Fabrication and application of PD-modified CFC immobilized with PNIPAM 103
6.1 Research background 103
6.2 Experiments 104
6.3 Results and discussion 105
6.3.1 Characterization of surface-modified CFCs 105
6.3.2 Fog harvesting efficiency of different surface-modified CFCs 108
6.3.3 Water dissipation adjustment using surface-modified CFCs 111
6.3.4 NIR-controllable valve using PNIPAM-PD/TiO2@ CFCs 112
6.4 Summaries 113
Chapter 7 Conclusions 126
References 129
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