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研究生:林奕辰
研究生(外文):Yi-Chen Lin
論文名稱:還原氧化石墨烯製備、性質與應用研究
論文名稱(外文):Preparation, Characteristics and Application of Reduced Graphene Oxide
指導教授:薛富盛薛富盛引用關係
指導教授(外文):Fuh-Sheng Shieu
口試委員:黃榮鑫林景崎薛康琳顏秀崗
口試委員(外文):Rong-Hsin HuangJing-Chie LinKan-Lin HsuehShiow-Kang Yen
口試日期:2019-07-18
學位類別:博士
校院名稱:國立中興大學
系所名稱:材料科學與工程學系所
學門:工程學門
學類:材料工程學類
論文種類:學術論文
論文出版年:2019
畢業學年度:107
語文別:英文
論文頁數:70
中文關鍵詞:硫化鎘石墨烯質子交換膜燃料電池
外文關鍵詞:CdSGraphenePEMFC
相關次數:
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本研究先使用Hummers 法,將石墨粉氧化成氧化石墨稀,並使用兩種還原方
式分別應用在:光觸媒之催化促進劑及質子交換膜燃料電池的吸濕材料。
第一部分:
使用超聲波方法,製備一系列不同重量比的硫化鎘和還原氧化石墨烯複合材
料,製備溫度70℃、20 分鐘。使用氨水作為鎘的絡合劑及氧化石墨烯的還原劑。
純硫化鎘顆粒具有差的結晶度並聚集成大顆粒尺寸。當氧化石墨稀摻入硫化鎘時,
清楚地觀察到在還原氧化石墨稀片上具有高結晶度的硫化鎘顆粒的均勻分散。所
製備的複合材料在可見光區域具有廣泛和強的光吸收,並且通過形成還原氧化石
墨稀和硫化鎘的異質結構,在可見光照射下顯示出對亞甲藍降解的顯著改善的光
催化活性。但是,過多的還原氧化石墨稀會屏蔽硫化鎘奈米顆粒表面的性位點的
光,因此限制了光催化效率的進一步提高。
第二部分:
使用聚四氟乙烯襯底的高壓釜製備還原氧化石墨稀,在100℃、12 小時。並
塗覆在陽極氣體擴散層做為吸濕材料改善質子交換膜燃料電池的性能。經傅里葉
轉換紅外光譜和X-射線繞射分析表明在還原氧化石墨烯中存在殘餘的含氧官能團。
場效發射式掃描電子顯微鏡及接觸角量測顯示還原氧化石墨烯均勻塗覆於氣體擴
散層及有最佳的接觸角117°。在氣體加濕溫度為25°C,45°C 和65°C 時,塗有陽
極氣體擴散層的還原氧化石墨烯膜電極組的功率密度比沒有還原氧化石墨烯的膜
電極組高30.92%,41%和36.20%。
In this study we use Hummers method to oxidize graphene then us two methods
reducing oxidized graphene (rGO) such ultrasonic method and thermal reduction. The
reduced graphene oxides were applied as a catalytic promoter photocatalysts and the
hygroscopic material PEMFC.
Part 1:
We report a facile ultrasonic method to prepare a series of CdS and reduced
graphene oxide composites with different weight ratios of graphene at temperature as
low as 70°C for 20 min by employing ammonia as a complexing agent of Cd2+ ions and
reducing agent of graphene oxide. Pure CdS particles had a poor crystallinity and
aggregated to large particles size. As GO was incorporated into CdS, a uniform
dispersion of CdS particles with high crystallinity on RGO sheets was clearly observed.
The as-prepared CdS/rGO composites have a wide and strong photo absorption in the
visible region and display a substantially improved photocatalytic activity for the
degradation of methylene blue under visible light irradiation by forming a
heterojunction of rGO and CdS. However, too much rGO will shield the light of the
active sites for the CdS nanoparticle surface and thus limit further improvement in the
photocatalytic efficiency.
Part 2:
We produced reduced graphene oxide by reduction of graphene oxide (GO) in
Teflon‐lined autoclave, maintained at 100°C for 12 hours, and coated on the anode gas
diffusion layer of a protonexchange membrane fuel cell to improve the cell
performance. Fourier transform infrared spectroscopy and X‐ray photoelectron
spectroscopy analysis showed the presence of residual oxygen‐containing functional
groups in rGO. Field‐emission scanning electron microscopy images revealed the
uniform and adequate coating of the GDLs with rGO. The wettability of rGOcoated
GDL was determined by the sessile drop method and has optimum contact angle 117°.
The power densities for the membrane electrode assembly with rGO coated on the
anode GDL were 30.92%, 41%, and 36.20% higher than those for the MEA without the
rGO coating at anode gas humidified temperatures of 25°C, 45°C, and 65°C,
respectively.
致謝..............................................................................................................................i
摘要.............................................................................................................................ii
Abstract........................................................................................................................iii
總目錄...........................................................................................................................iv
圖目錄...........................................................................................................................vi
表目錄...........................................................................................................................ix
Chapter 1.........................................................................................................................1
Introduction......................................................................................................................1
1.1 Graphene material.............................................................................................................1
1.2 Graphene Production Techniques................................................................................................1
(1) Synthesis on SiC Method.......................................................................................................1
(2) Chemical Vapor Deposition (CVD)...............................................................................................2
(3) Liquid-phase Exfoliation......................................................................................................2
(4) Reduced Graphene Oxide (rGO)..................................................................................................2
1.3 Introduction of Water Splitting...............................................................................................3
1.4 Types of Fuel cell............................................................................................................3
1.5 References....................................................................................................................5
Chapter 2........................................................................................................................11
Ultrasonic chemical synthesis of CdS-reduced graphene oxide nanocomposites with an enhanced visible light photoactivity..........11
Abstract.........................................................................................................................11
2.1 Introduction.................................................................................................................12
2.2 Experimental.................................................................................................................14
2.2.1 Material...................................................................................................................14
2.2.2 Synthesis of GO............................................................................................................14
2.2.3 Synthesis of CdS and the CdS/rGO composite material........................................................................14
2.2.4 Characterization...........................................................................................................14
2.2.5 Measurement of the photocatalytic degradation of MB........................................................................15
2.3 Results and Discussion.......................................................................................................16
2.3.1 Structure, morphology, and composition of CdS/rGO..........................................................................16
2.3.2 Chemical bonding of rGO/CdS................................................................................................17
2.3.3 Optical properties of rGO/CdS..............................................................................................18
2.3.4 Photodegradation of MB and the stability of CdS/rGO........................................................................19
2.3.5 Photocatalytic mechanisms..................................................................................................20
2.4 Conclusion...................................................................................................................21
2.5 References...................................................................................................................22
Chapter 3........................................................................................................................41
Reduced graphene oxide–coated anode gas diffusion layer for performance enhancement of proton-exchange membrane fuel cell.............................................................................................................................41
Abstract.........................................................................................................................41
3.1 Introduction.................................................................................................................42
3.2.Experimental.................................................................................................................44
3.2.1 Preparation of graphene oxide..............................................................................................44
3.2.2 Preparation of rGO and rGO-coated GDL......................................................................................44
3.2.3 Characterization...........................................................................................................44
3.2.4 Preparation of MEA.........................................................................................................44
3.2.5 Measurement of polarization curves.........................................................................................45
3.3 Results and Discussion.......................................................................................................45
3.3.1 Structure and composition of rGO...........................................................................................45
3.3.2 Physical characterization of rGO-coated GDL................................................................................46
3.3.3 Single-cell polarization test..............................................................................................47
3.4 Conclusion...................................................................................................................50
3.5 References...................................................................................................................51
Vita and Publication List........................................................................................................70
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