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  1. NTU Theses and Dissertations Repository
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請用此 Handle URI 來引用此文件: http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/41191
完整後設資料紀錄
DC 欄位值語言
dc.contributor.advisor張慶源
dc.contributor.authorTao-Ming Liuen
dc.contributor.author劉道明zh_TW
dc.date.accessioned2021-06-14T17:22:52Z-
dc.date.available2010-07-30
dc.date.copyright2008-07-30
dc.date.issued2008
dc.date.submitted2008-07-24
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36. Schrebler, R., P. Cury, C. Suaŕez, E. MunÕz, H. Goḿez and R. Coŕdova, Study of the electrochemical reduction of CO2 on a polypyrrole electrode modified by rhenium and copper_/rhenium microalloy in methanol media. J. Electroanal. Chem., 533(1-2), 167-175 (2002).
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dc.identifier.urihttp://tdr.lib.ntu.edu.tw/jspui/handle/123456789/41191-
dc.description.abstract隨著全球經濟的發展,所耗用之石化資源不斷的增加,也伴隨著汙染物的產生。其中以二氧化碳的排放為世界關注重點,所造成的全球暖化問題為最大議題之一。科學證據顯示人為活動為造成近百年來的全球暖化現象之主因。故CO2減量議題成為目前全球所關注的焦點之一。
本研究主要利用電解還原反應將CO2還原形成可再利用之能源 (如CH4、C2H6及CO) 及化工原料 (如C2H4及HCOOH)。所使用之還原程序有下列三種。(1) 電解還原程序:藉由電解水分子產生H+及電子之傳遞,將CO2選擇性還原生成CH4、C2H6、C2H4、CO及HCOOH;其氣相碳源產率達50%。(2) 光觸媒催化還原程序:利用改質之二氧化鈦光觸媒在不同光源波長下激發產生電子電洞對,可選擇性還原CO2為CH4及C2H4,氣相碳源產率約為10%。(3) 光電化學觸媒還原程序:合併電解還原與光觸媒還原程序使氣相碳原產率提升,可將CO2還原生成CH4、C2H4、C2H6、CO、HCOOH及副產物H2;其氣相碳源產率可達70%。利用此光電化學觸媒還原程序可選擇性還原CO2生成碳氫化合物等石化資源,一方面提供做為工業用原料,另一方面可以降低溫室氣體CO2排放問題,為減碳科技之新穎技術之一。
zh_TW
dc.description.abstractAlong with the prompt development of every country, two special problems are generated all over the world. The first problem is the increasing comsumption of energy and the other one is the deterious pollution of environment. There are many evidences showing that global warming is caused by human activity. Therefore, every country focuses on the emission of CO2 to the atmosphere from power plants, industries and so on.
The study investigated the application of reduction of carbon dioxide to useful chemicals via photo-electro-catalytic reduction (PECR) method. The first part of this study directly applied electrolysis reduction process (ER) to generate a certain mount of electron and hydrogen ion for selectively converting gaseous CO2 to hydrocarbons including methane (CH4), ethane (C2H6), ethylene (C2H4), carbon monoxide (CO) and formic acid (HCOOH). The yield of gaseous carbon species (Yc) other than CO2 can reach about 50%. For the second part, different modified catalysts were introduced in the photo-catalytic process (PCR) to reduce the gaseous CO2, giving Yc of about 10%. Finally, the first two reduction processes were combined to concert the CO2. This novel PECR process can convert carbon dioxide more efficiently, resulting in a high Yc of 73%. Thus the application of the proposed PECR process can not only reuse CO2 to reduce the global warming potential, but also produce useful chemicals for industrial usage. For those advantages, the PECR process may be a feasible technology in the future.
en
dc.description.provenanceMade available in DSpace on 2021-06-14T17:22:52Z (GMT). No. of bitstreams: 1
ntu-97-R95541117-1.pdf: 2207468 bytes, checksum: f4cf250b195b84044b0bcf99ed05fd91 (MD5)
Previous issue date: 2008
en
dc.description.tableofcontents中文摘要 i
英文摘要 ii
目錄 iii
圖目錄 vii
表目錄 xii
符號說明與縮寫說明 xiii
第一章 研究動機與目的 1
1.1 研究背景 1
1.2 研究目的 2
第二章 文獻探討 4
2.1 二氧化碳現況 4
2.1.1 大氣中二氧化碳排放現況 4
2.1.2 國際輿論 5
2.2 二氧化碳處理法 8
2.3 電解氧化還原理論 9
2.3.1 電壓電流影響 11
2.3.2 電極種類影響 11
2.3.3 電解質濃度與種類影響 12
2.3.4 溫度之影響 12
2.4 光觸媒氧化還原理論 16
2.5 光觸媒催化結合電化學以還原CO2之研究 21
2.5.1 光觸媒催化與電化學還原CO2之研究 21
2.5.2 太陽能光電化學觸媒法還原CO2之研究 23
第三章 研究方法 27
3.1 實驗材料與設備 27
3.1.1 反應系統 27
3.1.2 設備與藥品 31
3.2 系統測試 33
3.2.1 反應器前置測試 33
3.2.2 電解前置測試 33
3.3 觸媒製備 34
3.3.1 Cu/TiO2製備 34
3.3.2 TiNH400製備 34
3.3.3 觸媒分析方法 36
3.3.3.1 掃描式電子顯微鏡 36
3.3.3.2 能譜儀 36
3.3.3.3 穿透式電子顯微鏡 36
3.4 光源強度測試 37
3.5 光觸媒催化電解還原二氧化碳實驗 37
3.5.1 電解還原反應 37
3.5.2 光觸媒催化還原反應 38
3.5.3 光觸媒催化電解還原反應 39
3.6 儀器操作與產物分析 40
3.6.1 儀器操作條件 40
3.6.2 產物定性與定量 41
3.6.3 液相碳源分析 41
第四章 結果與討論 42
4.1 電解還原程序 42
4.1.1 離子強度 43
4.1.2 電解質種類 50
4.1.3 工作氣體 56
4.1.4 電解還原機制之探討 56
4.2 光觸媒催化還原程序 58
4.2.1 光還原反應 59
4.2.2 光觸媒催化還原反應 61
4.2.2.1 光源種類 61
4.2.2.2 光觸媒種類 64
4.2.3 光觸媒催化還原機制之探討 67
4.3 光觸媒催化電解還原反應 68
4.3.1 光電解還原反應 68
4.3.2 光觸媒催化電解還原反應 75
4.3.2.1 Na2CO3電解質組成之影響 75
4.3.2.2 光源種類之影響 85
4.3.2.3 光觸媒種類之影響 91
4.4 綜合討論 97
4.4.1 產率比較 97
4.4.2 氣相CO2去除率比較 106
4.4.3 總轉化率比較 106
4.4.4 pH比較 108
4.4.5 光觸媒溶液導電度比較 110
4.4.6 產物反應途徑與反應機制探討 111
第五章 結論與建議 113
5.1 結論 113
5.2 建議 115
參考文獻 117
附錄A 檢量線製作 121
附錄B 光觸媒成分含量百分比 132
附錄C GC-FID成分峰圖 133
附錄D 光源強度測試 134
附錄E ER、CPR、CPER產物熱值表 135
dc.language.isozh-TW
dc.subjectGreen-house gasen
dc.subjectpetroleumen
dc.subjectethyleneen
dc.subjectphoto-electro-catalsisen
dc.subjectphoto-catalysisen
dc.subjectelectrolysisen
dc.title應用光電化學觸媒法還原二氧化碳產製化學品之研究zh_TW
dc.titleReduction of CO2 to Produce Useful Chemicals via Photoelectrocatalystsen
dc.typeThesis
dc.date.schoolyear96-2
dc.description.degree碩士
dc.contributor.oralexamcommittee張章堂,謝哲隆
dc.subject.keyword溫室氣體,電解,光觸媒催化,光電化學觸媒催化,石化能源,乙烯,zh_TW
dc.subject.keywordGreen-house gas,electrolysis,photo-catalysis,photo-electro-catalsis,ethylene,petroleum,en
dc.relation.page137
dc.rights.note有償授權
dc.date.accepted2008-07-26
dc.contributor.author-college工學院zh_TW
dc.contributor.author-dept環境工程學研究所zh_TW
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