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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 張慶源(Ching-Yuan Chang) | |
dc.contributor.author | Kuan-Yu Liu | en |
dc.contributor.author | 劉冠郁 | zh_TW |
dc.date.accessioned | 2021-06-16T13:19:09Z | - |
dc.date.available | 2023-12-31 | |
dc.date.copyright | 2013-07-30 | |
dc.date.issued | 2013 | |
dc.date.submitted | 2013-07-26 | |
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/61928 | - |
dc.description.abstract | 因應我國能源自給之困難,本研究以高溫高壓觸媒床合成氣(CO及H2)重組反應產製液體燃料,以期未來能應用於生質物氣化產品合成氣之進一部利用,除了可解決能源問題外亦可降低環境之汙染。
本研究之實驗使用連續式高壓觸媒填充床(high pressure catalytic packed bed, HPCPB)將合成氣轉化為液體燃料。以自製比表面積達800 m2/g中孔性分子篩SBA-15(Santa Barbara amorphous-15)做為觸媒之擔體,批覆Mo2C觸媒於顆粒表面後,將使原本SBA-15之晶型結構稍微掩蓋,另觸媒表面鉬含量達20 wt.%仍具500 m2/g之高比表面積。研究結果顯示:觸媒床反應器中進行只填充SBA-15,並未產生合成氣之重組反應;而填充觸媒Mo2C/SBA-15後即有提高CO轉化之效果,且醇類產物之選擇性(selectivity, S)亦高。研究中探討鉬含量對合成氣重組之影響,結果顯示當鉬含量提升時,CO之轉化率(conversion of CO, XCO)可大幅之上升。另外亦針對其他重要操作參數之影響進行探討,包括:反應器溫度(T),壓力(P)及氣體流量(QG)。參考條件為:T = 523 K, P = 450 psi, QG = 60 mL min-1, 20% Mo2C/SBA-15觸媒量(mS) = 5 g,觸媒體積(VS) = 3.76 mL。實驗結果得知,反應溫度由473 K提升至573 K,XCO由10.76% 提高至59.75%,增加48.99%,但醇類產物之選擇性(SOH) 由92.32% 下降至13.81%,降低78.51%。而壓力參數設定由250 psi增高至450 psi時,並無顯著之影響,唯乙醇之産率(yield of ethanol (EtOH), YEtOH)由1.18%提高至1.52%,有些微之增加。合成氣之進氣流量影響氣體之空間流速(gas hourly space velocity, GHSV = QG/VS),GHSV之倒數即氣體在反應器中與觸媒之接觸時間。當QG由90降低至30 mL min-1時,XCO雖可由24.82% 提高至49.15%,但會使高碳數之醇類分解為低碳數之烷類及醇類,因而高碳數醇類產物之選擇性由5.32%降低至3.34%。故在氣體流量之選擇上,須考慮目標產物為何,進而對其做一適切之選擇。另本實驗之觸媒失活試驗結果顯示,觸媒之使用時間在96小時內仍可維持其80%以上之活性。且由使用前後觸媒之掃描式電子顯微鏡(scanning electronic microscope, SEM)觀察結果,可知觸媒之失活原因在於觸媒表面之積碳所致。 | zh_TW |
dc.description.abstract | In order to reduce the stress of energy demand and pollution, reforming of syngas (CO and H2), which may be obtained from biomass gasification process, can produce liquid fuel and reduce green house gases (GHGs) emission.
This study examined the feasibility and operation performance of reforming of syngas via high pressure catalytic packed bed (HPCPB) process. Mesoporously molecular sieves of Santa Barbara amorphous-15 (SBA-15), which has small paticle size of 31.75 μm and high BET (Brunauer- Emmett- Teller) suffice area of 800 m2/g was used as the support of catalyst. Catalytic species of Mo2C was well dispersed on the support. The blank experiment indicated no reavtion between SBA-15 and syngas. The Mo2C catalyst containg Mo 20 wt.% exhibits significant conversion of CO (XCO). Main system parameters investigated include temperature (T), pressure (P) and the influent gas flow rate (QG). In addition to XCO, the production rate, selectivity and yield were also elucidated. The T and QG have more significant influences on the system performance than P. The result shows a higher T gives higher XCO, while lower selectivity of alcohols. A low QG, which means gas has long contact time with catalyst, improves the XCO, however it can cause the decomposition of butnol to low carbon content products. To select suitable QG, one should consider which alcohol product is the target. The increase of pressure from 250 to 450 psi examined in this study has no obvious enhancing effect as compared to other operation parameters. The catalytic deactivation test shows that the catalyst can maintain 80% activity after 96 hr. The SEM observation indicated the carbon accumulation on the catalyst surface, which may thus cause the deactivation. | en |
dc.description.provenance | Made available in DSpace on 2021-06-16T13:19:09Z (GMT). No. of bitstreams: 1 ntu-102-R00541119-1.pdf: 4154765 bytes, checksum: f9996243aa4be2c1bb67baa7d7cb98a2 (MD5) Previous issue date: 2013 | en |
dc.description.tableofcontents | 目錄
目錄 iv 圖目錄 vi 表目錄 x 符號說明 xii 第一章 緒論 1 1.1研究緣起 1 1.2研究內容 2 1.3研究目標 2 第二章 文獻回顧 6 2.1合成氣 6 2.2合成氣轉製燃料 6 2.2-1反應機制 9 2.2-2反應條件 12 2.2-3合成氣於觸媒表面之反應 15 2.3觸媒 18 2.3-1擔體之選用:中孔性分子篩SBA-15 18 2.3-2觸媒之選用:鉬基(Mo-based)觸媒 19 2.4生質酒精之經濟效益 20 第三章 實驗設備與研究方法 24 3.1研究架構 24 3.2觸媒合成 26 3.2.1實驗材料與設備 26 3.2-2合成步驟 27 3.2.3分析項目及原理 30 3.3高溫高壓反應實驗之材料與分析設備 31 3.3-1實驗材料 31 3.3-2相層析儀‐熱傳導偵測器(GC‐TCD, China Chromatography 8900) 32 3.3-3氣相層析儀‐火焰梨子偵測器(GC‐FID) 33 3.3.4溫度計及壓力計 36 3.4連續式高溫高壓反應實驗 36 3.5分析項目與評估方法 37 第四章 結果與討論 41 4.1觸媒之特性分析 41 4.1-1觸媒之物理特性分析 41 4.1-2 SEM-EDS掃描圖像 42 4.1-3 SEM拍攝結果 45 4.1-4 XRD定性繞射分析 49 4.2基礎背景試驗 54 4.3高溫高壓觸媒床程序 (High pressure catalytic packed bed process, HPCPB process) 55 4.3-1觸媒種類(Mo content)之影響 55 4.3-2溫度(Temperature)之影響 64 4.3-3壓力(Pressure)之影響 75 4.3-4 總氣體流量(QG)之影響 81 4.4觸媒失活試驗 95 第五章 結論與建議 97 5.1結論 97 5.2建議 98 參考文獻 100 附錄 A 分子篩之比較及命名 A-1 附錄 B 多孔性觸媒粒徑分佈 B-1 附錄 C 觸媒吸脫附曲線 C-1 附錄 D 檢量線 D-1 附錄 E 原始數據 E-1 | |
dc.language.iso | zh-TW | |
dc.title | 鉬基多孔性觸媒應用於合成氣產製烷類及醇類之研究 | zh_TW |
dc.title | Production of Alkanes and Alcohols from Syngas over
Porous Mo-based Catalyst | en |
dc.type | Thesis | |
dc.date.schoolyear | 101-2 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 章裕民(Yu-Min Chang),陳奕宏(Yi-Hung Chen),謝哲隆(Je-Lueng Shie) | |
dc.subject.keyword | 合成氣,液體燃料,連續式高壓觸媒填充床,SBA-15,Mo2C,合成氣重組反應,失活試驗, | zh_TW |
dc.subject.keyword | Syngas,liquid fuel,high pressure catalytic packed bed,SBA-15,Mo2C,deactivation, | en |
dc.relation.page | 122 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2013-07-26 | |
dc.contributor.author-college | 工學院 | zh_TW |
dc.contributor.author-dept | 環境工程學研究所 | zh_TW |
顯示於系所單位: | 環境工程學研究所 |
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