(100.25.42.117) 您好!臺灣時間:2021/04/21 17:09
字體大小: 字級放大   字級縮小   預設字形  
回查詢結果

詳目顯示:::

我願授權國圖
: 
twitterline
研究生:張宗盛
研究生(外文):CHANG,TSUNG-SHENG
論文名稱:質子交換膜燃料電池 C-B-Pt、C-B-Pd 電極觸媒材料之開發
論文名稱(外文):Development of C-B-Pt、C-B-Pd Electrode Materials Catalyst for Proton Exchange Membrane Fuel Cells
指導教授:劉鳳錦
指導教授(外文):LIU,FENG-CHIN
口試委員:洪儒熙薛康琳方良吉張文昇
口試委員(外文):HUNG,JU-HSIHSUEH,KANG-LINFANG,LIANG-CHICHANG,WEN-SHENG
口試日期:2013-06-24
學位類別:碩士
校院名稱:國立聯合大學
系所名稱:化學工程學系碩士班
學門:工程學門
學類:化學工程學類
論文種類:學術論文
論文出版年:2013
畢業學年度:101
語文別:中文
論文頁數:142
中文關鍵詞:燃料電池水熱合成法碳硼觸媒觸煤活性
外文關鍵詞:Fuel cellHydrothermal SynthesisBoron doped carbonCatalytic activity
相關次數:
  • 被引用被引用:1
  • 點閱點閱:141
  • 評分評分:系統版面圖檔系統版面圖檔系統版面圖檔系統版面圖檔系統版面圖檔
  • 下載下載:6
  • 收藏至我的研究室書目清單書目收藏:0
本研究主要目的在於開發適用於燃料電池的新型觸媒。以碳硼為載體,利用水熱合成法製備碳-硼-鉑合金觸媒(C-B-Pt)與碳-硼-鈀合金觸媒(C-B-Pd),期望提升觸媒分散性及活性。實驗上藉由改變碳硼基材條件如:碳粉pH值、硼酸含量、實驗設備裝置及熱處理鍛燒溫度等因素,找出最佳之碳硼基材之製備條件。後續輔以添加貴金屬六氯鉑酸與氯化鈀來探討其效能,期望獲得高活性、高抗腐蝕性之碳硼觸媒來降低白金貴金屬之使用成本。本實驗製得之碳硼觸媒,利用CA、FE-SEM、EDS、FT-IR、XRD及RDE等儀器來測定,探討觸媒親疏水性、觸媒表面型態結構、元素分析與分佈情形、觸媒鍵結、觸媒金屬晶相和觸媒活性等相關特性。
實驗結果顯示, XC-72R碳粉與硼酸之重量最佳化配比為1:5.2,於鐵氟龍容器水熱合成後,加以鍛燒熱處理,具有最佳之碳硼載體。C-B-Pt salt5% 經450℃鍛燒3小時後,在含氧0.5M 硫酸溶液中,掃描速率固定為5mV/s,轉速為900rpm操作循環伏安法,具有最佳之觸媒活性及高比電流密度-18.8 (mA/cm2/g Pt)。

關鍵字:燃料電池、水熱合成法、碳硼觸媒、觸煤活性

This study aims to develop a suitable new type of catalyst for fuel cell. It takes carborane as the support, uses hydrothermal synthesis technology to prepare carboran-platinum alloy catalysts (C-B-Pt) and carboran-palladium alloy catalysts (C-B-Pd) to obtain better catalyst dispersion and reaction activity. To find the best catalyst preparation condition, experimental factors under investigation are:carbon pH value,boric acid content, type of preporation methods, heat-treated calcination temperature, etc. Precious metals salts, such as hexachloroplatinate and palladium chloride were then added on the carboranes. These catalysts are expect to have high activity, high corrosion resistance, and lower cost than platinum catalyst. The generated carborane catalyst from this study will be examined by contact angle for hydrophobicity, FE-SEM for surface morphology, EDS for element analysis, FT-IR for element distribution, XRD for crystal phase identification, and RDE for electrochemical activity. The result suggests that calcination with XC-72R carbon and boric acid at weight ratio of 1:5.2 in Teflon containers would obtained the optimum carborane support. After calcinations of 3 hours at 450℃, of the C-B-Pt salt 5%. The catalyst activity was evaluated by rotating disk electrode with electrode potential scan rate at 5mV/s in 0.5 M sulfuric acid saturated with oxygen, atelectrode rotating speed of 900 rpm. The optimum current density of 18.8 (mA/cm2/g Pt) was obtained.

Keywords:Fuel cell;Hydrothermal Synthesis;Boron doped carbon;Catalytic activity

摘要 i
Abstract ii
目 錄 ii
圖目錄 vii
表目錄 xiii
第一章 緒論 1
1.1 前言 1
1.2 研究動機 2
第二章 原理與文獻回顧 3
2.1 燃料電池簡介 3
2.1.1 燃料電池發展史 3
2.1.2 燃料電池分類 4
2.2 質子交換膜燃料電池(PEMFC)簡介與關鍵元件 6
2.2.1 觸媒 10
2.2.2 質子交換膜 12
2.2.3 電極 14
2.2.4 雙極流場板 15
2.3 應用於燃料電池之碳載體-碳材前處理 16
2.4 電池電化學特性 18
2.4.1 循環伏安法 18
2.4.2 極化曲線 20
2.5 旋轉圓盤電極原理簡介 22
2.6 碳硼合金觸媒 23
2.6.1 硼的簡介 23
2.6.2 碳化硼結構與材料 25
2.6.3 碳化硼聚合物發展史 27
2.6.4 碳化硼合金之應用與開發 29
第三章 實驗設備與研究方法 32
3.1 實驗藥品 32
3.2 實驗設備 33
3.3 實驗架構 34
3.4 實驗步驟 35
3.4.1 碳硼載體製備 35
3.4.1.1 碳粉前處理 35
3.4.1.2 碳硼載體基材製備 37
3.4.2 碳硼合金觸媒製備 40
3.5 特性分析 44
3.5.1 接觸角量測儀 44
3.5.2 冷場發射掃描式電子顯微鏡 45
3.5.3 能量散佈光譜儀 47
3.5.4 傅立葉轉換紅外線光譜儀 48
3.5.5 X-ray繞射分析儀 49
3.5.6 旋轉圓盤電極 50
第四章 結果與討論 52
4.1 親疏水性分析 52
4.2冷場發射掃描式電子顯微鏡分析 57
4.3元素分析 64
4.4 傅立葉轉換紅外線光譜儀分析 70
4.5 X-ray繞射分析儀分析 73
4.6旋轉圓盤電極觸媒活性分析 76
4.6.1 碳硼觸媒 76
4.6.1.1 合成製程差異探討 77
4.6.1.2 硼酸含量探討 78
4.6.1.3 碳粉pH值探討 79
4.6.2 C-B-Pt、C-B-Pd觸媒 83
4.6.2.1 RDE掃描-硫酸水溶液中導入氧氣 84
4.6.2.2 RDE掃描-硫酸水溶液中導入氮氣 97
第五章 結論與未來展望 118
5.1結論 118
5.2未來展望 120
第六章 參考文獻 121

1.A. Garsuch﹐R. Yang﹐A. Bonakdarpour and J.R. Dahn﹐“ The effect of boron doping into Co-C-N and Fe-C-N electrocatalysts on the oxygen reduction reaction ” ﹐Electrochimica Acta , Vol.53﹐P.2423~2429 (2008).
2.S. Li﹐L. Zhang﹐J. Kim﹐M. Pan﹐Z. Shi and J. Zhang﹐“ Synthesis of carbon-supported binary FeCo–N non-noble metal electrocatalysts for the oxygen reduction reaction ” ﹐Electrochimica Acta , Vol.55﹐P.7346~7353 (2010).
3.Y.J. Si﹐C.G. Chen﹐W. Yin and H. Cai, “ Electrocatalytic activity of non-precious metal catalyst Co–N/C toward oxygen reduction reaction ”
﹐Chinese Chemical Letters﹐Vol.21﹐P.983~986(2010).
4.J. Chen﹐Z.H. Zhu﹐S. Wang﹐Q. Ma﹐V. Rudolph and G.Q. Lu ﹐“ Effects of nitrogen doping on the structure of carbon nanotubes (CNTs) and activity of Ru/CNTs in ammonia decomposition ” ﹐ Chemical Engineering Journal﹐Vol.156﹐P.404~410 (2010).
5.C. W.B. Bezerra﹐L. Zhang﹐K. Lee﹐H. Liu﹐A. L.B. Marques﹐E.P. Marques﹐H. Wang and J. Zhang﹐“ A review of Fe–N/C and Co–N/C catalysts for the oxygen reduction reaction ” ﹐Electrochimica Acta﹐ Vol.53﹐P.4937~4951(2008).
6.Y. Mu﹐M. Wang and D. Yu﹐“ Synthesis of Ti(CN) powders by combustion reaction from Ti powder and a novel carbon–nitrogen precursor ” ﹐Int. Journal of Refractory Metals and Hard Materials﹐ Vol.29﹐P.326~328(2011).
7.K.Sopin and W.Daud﹐“ Challenges and future developments in proton exchange membrane fuel cell ” ﹐Renewable Energy ﹐Vol.31 ﹐P.719~727(2006).
8.黃鎮江﹐“ 燃料電池 ” ﹐第二版﹐台灣﹐全華圖書出版社 (2005).
9.余佩蓉﹐“ 質子交換膜燃料電池膜電極組製備及其對電池性能影響之研究 ” ﹐國立聯合大學碩士論文(2009).
10.張凱硯﹐“ 質子交換膜燃料電池CNX電極材料之開發 ” ﹐國立聯合大學碩士論文(2012).
11.顏妙妤﹐“ 以電化學脈衝法沉積觸媒於燃料電池氣體擴散層之研究 ” ﹐逢甲大學碩士論文(2007).
12.S. Litster1 avd G. McLean﹐“ PEM fuel cell electrodes ” ﹐Journal of Power Sources﹐Vol.130﹐P.61~76 (2004).
13.J. M. J. Leo and M. N. Mugerwa﹐“ Fuel Cell Systems ” ﹐ Kluwer Academic / Plenum Publishers (1993).
14.陳國袖﹐“ Ni-P/TiO2/C合金觸媒製備及對質子交換膜燃料電池之應用研究 ” ﹐國立聯合大學碩士論文(2011).
15.C.C. Huang﹐H.S. Li and C.H. Chen﹐“ Effect of surface acidic oxides of activated carbon on adsorption of ammonia ” ﹐Journal of Hazardous Materials﹐Vol.159﹐P.523~527(2008).
16.Ryan O´Hayre﹐“ Fuel cell fundamentals ” (2008).
17.吳浩青﹐“ 電化學動力學 ”﹐初版﹐台北﹐科技圖書出版社(2001).
18.W. Ding﹐S. Ding﹐S. Zheng﹐M. Xie﹐L. Peng and X. Guo﹐“ One-pot synthesis of boron-doped mesoporous carbon with boric acid as a multifunction reagent ” ﹐Microporous and Mesoporous Materials ﹐Vol.142﹐P. 609~613(2011).
19.C. Barboiu﹐B. Sala﹐S. Bec﹐S. Pavan﹐E. Petit﹐Ph. Colomban﹐J. Sanchez﹐S. de Perthuis and D. Hittner﹐“ Structural and mechanical characterizations of microporous silica–boron membranes for gas separation ” ﹐Journal of Membrane Science﹐Vol.326 ﹐P.514~525(2009).
20.O.M. Moon﹐B.C. Kang﹐S.B. Lee and J.H. Boo﹐“ Temperature effect on structural properties of boron oxide thin films deposited by MOCVD method ” ﹐Thin Solid Films ﹐Vol.464~465 ﹐P.164~ 169(2004).
21.Y. Jeong and T.C. Mike Chung﹐“ Mono-dispersed transition metal nanoparticles on boron-substituted carbon support and applications in hydrogen storage ” ﹐CARBON﹐Vol. 49 ﹐P.140~146 (2011).

22.S. Mondal and A.K. Banthia﹐“ Low-temperature synthetic route for boron carbide ” ﹐Journal of the European Ceramic Society ﹐Vol.25﹐ P.287~291(2005).
23.R.K. Dash﹐A. Nikitin and Y. Gogotsi﹐“ Microporous carbon derived from boron carbide ” ﹐Microporous and Mesoporous Materials ﹐Vol.72 ﹐P.203~208(2004).
24.J. Romanos﹐M. Beckner﹐D. Stalla﹐A. Tekeei﹐G. Suppes﹐S. Jalisatgi﹐M. Lee﹐F. Hawthorne﹐J.D. Robertson﹐L. Firlej﹐B. Kuchta﹐C. Wexler﹐P. Yu and P. Pfeifer﹐“ Infrared study of boron–carbon chemical bonds in boron-doped activated carbon ”﹐CARBON ﹐Vol.54﹐P.208~214(2013).
25.C.K. Acharya﹐W. Li , Z. Liu﹐G. Kwon﹐C. Heath Turner﹐Alan M. Lane﹐David Nikles﹐Tonya Klein and Mark Weaver﹐“ Effect of boron doping in the carbon support on platinum nanoparticles andcarbon corrosion ” ﹐Journal of Power Sources ﹐Vol.192 ﹐P.324~329 (2009).
26.T. Wang , C.X. Zhang﹐X. Sun﹐Y. Guo﹐H. Guo﹐J. Tang﹐H. Xue﹐M.Z. Liu﹐X.X. Zhang﹐L. Zhu﹐Q.Q. Xie and J.P. He﹐“ Synthesis of ordered mesoporous boron-containing carbon films and their corrosion behavior in simulated proton exchange membrane fuel cells environment ” ﹐Journal of Power Sources﹐ Vol.212﹐P.1~12(2012).

27.H.W. Bai﹐G. Wen﹐X.X. Huang﹐Z.X. Han﹐B. Zhong﹐Z.X. Hu and X.D. Zhang﹐“ Synthesis and structural characterization of SiBOC ceramic fibers derived from single-source polyborosiloxane ” ﹐ Journal of the European Ceramic Society ﹐Vol.31 ﹐P.931~940 (2011).
28.H. Aoki﹐T. Masuzumi﹐M. Hara﹐Z. Lu﹐D. Watanebe﹐C. Kimura and T. Sugino﹐“ Influence of the methyl group on the dielectric constant of boron carbon nitride films containing it ” ﹐Diamond & Related Materials ﹐Vol.19﹐ P.1437~1440 (2010).
29.L.M. Babkov﹐I.I. Gnatyuk and S.V. Trukhachev﹐“ Investigation of
4′-n-alkyl-4-cyanobiphenyls structure features by IR spectroscopy methods” ﹐Journal of Molecular Structure﹐Vol.744~747﹐P.425~432
(2005).
30.S.J. Park and J.M. Park﹐“ Preparation and characteristic of platinum catalyst deposited on boron-doped carbon nanotubes ” ﹐Current Applied Physics ﹐Vol.12 ﹐P.1248~1251 (2012).
31.F.X. Jiang﹐F.F. Ren﹐W.Q. Zhou﹐Y.K. Du﹐J.K. Xu﹐P. Yang and C.Y. Wang﹐“ Free-standing poly[poly(N-vinyl carbazole)]-supported Pt-based catalysts with enhanced performance for methanol electro-oxidation in alkaline medium ” ﹐Fuel ﹐Vol.102 ﹐P.560~566 (2012).

32.J. Hannauer﹐U.B. Demirci﹐C. Geantet﹐J.M. Herrmann and P. Miele﹐“ Transition metal-catalyzed dehydrogenation of hydrazine borane N2H4BH3 via the hydrolysis of BH3 and the decomposition of N2H4 ” ﹐international journal of hydrogen energy ﹐Vo1.37﹐P.10758~10767(2012).
33.T. Arunagiri, T.D. Golden and O. Chyan﹐“ Study of palladium metal particle deposition on the conductive diamond surface by XRD, XPS and electrochemistry ” ﹐Materials Chemistry and Physics ﹐Vo1.92 ﹐P.152~158(2005).
34.N. Meyer﹐K. Bekaert﹐D. Pirson﹐M. Devillers and S. Hermans﹐“ Boron nitride as an alternative support of Pd catalysts for the selective oxidation of lactose ” ﹐Catalysis Communications ﹐Vo1.29 ﹐P.170~174(2012).
35.M. Kakiage﹐Y. Tominaga﹐I. Yanase and H. Kobayashi﹐“ Synthesis of boron carbide powder in relation to composition and structural homogeneity of precursor using condensed boric acid–polyol product ” ﹐Powder Technology ﹐Vo1.221 ﹐P.257~263 (2012).
36.胡啟章﹐“ 電化學原理與方法 ” ﹐二版﹐台灣﹐五南圖書出版社(2002).
37.H.L. Guo and Q.M. Gao﹐“ Boron and nitrogen co-doped porous carbon and its enhanced properties as supercapacitor ” ﹐Journal of Power Sources ﹐Vo1.186 ﹐P.551~556 (2009).

QRCODE
 
 
 
 
 
                                                                                                                                                                                                                                                                                                                                                                                                               
第一頁 上一頁 下一頁 最後一頁 top
無相關期刊
 
系統版面圖檔 系統版面圖檔