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研究生:姚彥丞
研究生(外文):Yen-Chen Yao
論文名稱:塑膠廢棄物催化裂解產能效率與裂解油物種特性變化之評估研究
論文名稱(外文):Evaluation of energy conversion efficiency and speciation characteristics of pyrolytic oil in catalytic pyrolysis of plastic wastes
指導教授:江康鈺江康鈺引用關係
學位類別:碩士
校院名稱:國立中央大學
系所名稱:環境工程研究所
學門:工程學門
學類:環境工程學類
論文出版年:2017
畢業學年度:105
語文別:中文
論文頁數:195
中文關鍵詞:生質塑膠塑膠廢棄物熱裂解催化裂解
外文關鍵詞:Biodegradable plasticPlastic wastePyrolysisCatalytic pyrolysis
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本研究應用流體化床催化裂解反應系統,探討不同種類之塑膠廢棄物,在控制熱裂解反應溫度560~580℃及添加5~15%之礦物型催化劑(沸石)條件下,共同熱裂解轉換能源之效率與裂解油物種特性之變化。研究探討之塑膠廢棄物種類,主要包括聚乳酸生質塑膠(Polylactic Acid, PLA)、聚對苯二甲酸乙二酯(Polyethylene terephthalate, PET)及聚苯乙烯(Polystyrene, PS),試驗規劃之摻混比例介於0%~30%。此外,不同塑膠廢棄物共同熱裂解之協同效應與反應動力特性,亦是本研究探討的重點。研究結果顯示,試驗之PLA反應活化能最高,約為258 kJ/mole,而PS之反應活化能最低,約為170 kJ/mole。且當共同裂解反應時,試驗之反應活化能,隨PET或PS之摻混比例增加,而有明顯降低之趨勢。亦即試驗之塑膠廢棄物在共同熱裂解反應過程,具有協同反應之效果。根據熱裂解產油率之分析結果顯示,PLA的產油率約為14.5%,隨PET或PS摻混比例增加而有增加之現象,其中尤以30%之PET添加比例最為明顯,其共同熱裂解之產油率增加至21%。若進一步考量熱解油中輕質油(light fraction)及重質油(heavy fraction)之比例特性,則明顯可知PLA與30%之PET或PS共同熱裂解,其輕質油產率分別由5.85%增加至10.95%及8.4%。添加催化劑之分析結果顯示,當添加5%~10%催化劑試驗,熱解油產率約從21%增加至22.63%,且其重質油之產率有降低之趨勢。根據裂解油之物化特性分析結果顯示,裂解油O/C比隨PET或PS摻混比例之增加而降低,約從1.0降低至0.5,此有助於減緩裂解油老化現象發生的潛勢。根據共同熱裂解產生之熱解油官能基分析結果顯示,輕質油之含氧官能基物質,逐漸轉變為支鏈或環狀官能基物質。此外,裂解油之含氮與含硫量,亦隨著共同裂解或催化裂解之反應,而有降低的趨勢,亦即後續熱解油之燃料應用時,將可有效降低污染物之排放潛勢。
This research aims to evaluate the energy conversion efficiency and speciation characteristics of pyrolytic oil in catalytic pyrolysis of plastic wastes by using fluidized bed reactor with controlled at pyrolysis temperature 560~580℃ and 5~15% mineral catalyst (zeolite) addition. The plastic wastes used in this research were including Polylactic Acid, (PLA), Polyethyleneterephthalate (PET), and Polystyrene (PS), respectively. Blending ratio of PET or PS was controlled at 0%~30%. Synergistic effect and kinetics characteristics in co-pyrolysis of plastic wastes were also discussed. The analysis results of activation energy of tested plastic wastes indicated that PLA got the higher activation energy (258 kJ/mole) than that of PS (170 kJ/mole). Meanwhile, activation energy of mixed plastic wastes was decreased with an increase in PET and/or PS addition. It implied that the synergistic effect was occurred at different PET or PS blending and could promote PLA cracking into small molecular. According to the results of pyrolytic oil yield from PLA, the pyroltic oil production was approximately 14.5% and oil yield was increased to 21% as PET blending ratio was increasing to 30%. Based on the yield results of light and heavy fraction of pyrolytic oil produced from mixed plastic wastes, in the case of PET or PS blending, yield of light oil fraction was increased from 5.85% to 10.95% and 8.4%, respectively. On the other hand, tested catalyst could slightly increase pyrolytic oil yield from 21% to 22.62% with catalyst addition ratio increasing from 5% to 10%. However, heavy fraction of pyrolytic oil was significantly decreased with an increase in catalyst addition. Based on the results of characteristics of pyrolytic oil, the O/C ratio of pyrolytic oil was decreased from 1.0 to 0.5 with an increased in PET or PS addition. It implied that pyrolytic oil produced from blended PET or PS could prevent the aging of pyrolytic oil during its storage or transportation. According to the analysis results of functional group in pyrolytic oil, light fraction of pyrolytic oil containing oxygenated functional group will convert to that of oil containing branched and/or aromatic functional group. The nitrogen and sulfur contents of pyrolytic oil were also decreased with PET or PS blending and tested catalyst addition. It could reduce significantly the air pollutants emission when it applied to alternative fuel application.
摘要 i
Abstract ii
誌謝 iv
目錄 v
圖目錄 ix
表目錄 xii
第一章 前言 1
第二章 文獻回顧 5
2-1 塑膠處理現況 5
2-2 熱裂解 8
2-2-1 熱裂解產物 11
2-2-2 熱裂解產物影響因素 13
2-3 裂解油特性與改質方法 31
2-3-1 裂解油特性分析 31
2-3-2 提昇裂解油穩定性之物理方法 36
2-3-3 提昇裂解油穩定性之化學方法 38
2-3-4 裂解油之老化評估 41
第三章 研究材料與方法 45
3-1 研究材料 46
3-1-1 原料之基本特性分析 46
3-1-2 催化劑之基本特性分析 46
3-2 試驗方法 46
3-2-1 原料之動力學分析 46
3-2-2 試驗設備 48
3-2-3 操作條件 49
3-2-4 試驗步驟 50
3-3 分析項目與方法 51
3-3-1 塑膠原料 51
3-3-2 催化劑 54
3-3-3 熱裂解產物 55
第四章 結果與討論 59
4-1 試驗材料之基本特性分析 59
4-1-1 塑膠原料之基本特性分析結果 59
4-1-2 催化劑之基本特性分析結果 60
4-1-3 熱重損失之分析結果 61
4-2 熱裂解產物之分析結果 68
4-2-1 熱裂解試驗之重覆分析結果 68
4-2-2 熱裂解產物之質量平衡 70
4-2-3 PET與PS摻混比例對熱裂解產物量之影響 78
4-2-4 添加催化劑對裂解產物產量之影響 83
4-3 熱裂解產物之特性分析 85
4-3-1 裂解油元素分析結果 85
4-3-2 裂解油官能基鑑定分析結果 92
4-3-3 氣體組成分析結果 103
4-3-4 催化劑對產物特性之影響 111
4-4 裂解產物之能源分析結果 126
4-4-1 添加PET/PS對裂解產物高位發熱量之影響 126
4-4-2 添加催化劑對裂解產物高位發熱量之影響 131
4-5 產能效率評估 132
4-5-1 碳分佈 132
4-5-2 能源密度 138
第五章 結論與建議 147
5-1 結論 147
5-1-1 不同塑膠與摻混比例對受熱行為與活化能之影響結果 147
5-1-2 不同塑膠與摻混比例對裂解產物之影響結果 147
5-1-3 添加催化劑對裂解產物之影響結果 148
5-1-4 摻混不同塑膠與添加催化劑對油品特性分析之影響結果 149
5-2 建議 149
參考文獻 151
附錄 163

附錄一、摻混不同塑膠及添加催化劑對產物量之影響 164
附錄一、摻混不同塑膠及添加催化劑對產物量之影響(續) 165
附錄二、PLA之氣體體積變化 166
附錄三、PS之氣體體積變化 166
附錄四、PLA90%+PET10%之氣體體積變化 167
附錄五、PLA80%+PET20%之氣體體積變化 167
附錄六、PLA70%+PET30%之氣體體積變化 168
附錄七、PLA90%+PS10%之氣體體積變化 168
附錄八、PLA80%+PS20%之氣體體積變化 169
附錄九、PLA70%+PS30%之氣體體積變化 169
附錄十、PLA70%+PET25%+PS5%之氣體體積變化 170
附錄十一、PLA70%+PET20%+PS10%之氣體體積變化 170
附錄十二、PLA70%+PET15%+PS15%之氣體體積變化 171
附錄十三、PLA70%+PET30%+5% catalyst之氣體體積變化 171
附錄十四、PLA70%+PET30%+10% catalyst之氣體體積變化 172
附錄十五、PLA70%+PET30%+15% catalyst之氣體體積變化 172
附錄十六、校正前氣體重量彙整表 173
附錄十六、校正前氣體重量彙整表(續) 174
附錄十七、校正因子與校正後氣體重量彙整表 175
附錄十七、校正因子與校正後氣體重量彙整表(續) 176
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