臺灣博碩士論文加值系統

隨著全球人口持續增加，不僅增加對於能源的消耗和廢棄物產出相對增加，目前透過廢棄物資源化(Waste to Energy)技術處置，被認為是具經濟可行和環境永續性。在解決廢棄物的問題同時再生能源達到廢棄物再利用。
塑膠是最廣泛地使用且多用途之材料。由於需求增加，全球塑膠產量在2017年持續增長至3.48億噸。由於其物理化學穩定性和非生物降解性，廢塑膠的處理被認為是一個嚴重的問題。利用廢塑膠是由碳氫化合物所組成，將廢塑膠作為產氫原料，藉由熱處理技術產生合成氣，進一步藉由觸媒催化提高產氫效率。然而，在廢塑膠產氫觸媒卻容易發生金屬燒結和碳沉積而逐漸失活或嚴重的碳沉積造成反應器堵塞，影響觸媒壽命及催化效率。
為了改善上述問題，本研究透過合成蛋黃型殼核結構觸媒，以鎳作為活性相核，以具氧化還原能力的CeO2、CeO2-ZrO2包覆形成功能型外殼，應用於廢塑膠氣化產氫。在第一部份模擬廢塑膠氣化合成氣評估觸媒催化能力，在殼核結構情況下，改善只含鎳核反應發生金屬燒結失活的問題及形成顆粒小且高分散的活性相鎳，因此具有83%的高甲烷轉化率及高催化穩定性。在第二部份甲烷裂解反應模擬高積碳環境，以Ni@CeO2-ZrO2改善Ni@CeO2因CeO2熱穩定性差使觸媒結構不穩定，發生燒結及碳沉積失活問題。進一步以CTAB作為開孔劑，改善觸媒催化能力，以Ni@CeO2-ZrO2-1-0.5為最佳觸媒參數，有將近60%之甲烷轉化率且反應1小時均未失活。第三部份以二階段流體化床氣化廢PE催化產氫實驗中，不同觸媒結構對催化影響中，以蛋黃型殼核觸媒最具優勢，由於其具有殼核結構外，殼核之間的空隙提供異相催化中均勻的反應環境，充分暴露其活性位點及高比表面積因此有最佳產氫量達730.6 mmol/h-g。

As the global population continues to increase, it not only increases the demand for energy but also produces excessive waste. Currently, Waste to Energy is a widely promoted concept, which is considered to be economically viable and environmentally sustainable. This technology not only to solve waste management but also produce renewable energy to achieve waste recycling.
Plastics are one of the most widely-used and multi-purpose materials. Due to increasing demand, global plastic has continuously grown to 348 million tons in 2017. The treatment of waste plastics is regarded as a serious problem due to its physiochemical stability and non-biodegradation. Waste plastics are composed of hydrocarbons. We can use it as hydrogen production materials. Using heat treatment technology to produce syngas further improve hydrogen production efficiency by catalyst catalysis. However, in the production of hydrogen catalysts from waste plastics have several problems. Metal sintering and carbon deposition are prone to gradual deactivation or severe carbon deposition causing reactor blockage, affecting catalyst life and catalytic efficiency.
In order to solve the problem, we synthesis yolk-shell structure catalyst, which uses nickel as an active phase and redox characteristic ceria-zirconia mixed metal oxide is used as the functional shell layer. The catalyst is applied to produce hydrogen from waste plastics gasification. In the first part, we simulated waste plastic gasification syngas to evaluate catalyst catalytic ability. under core-shell structure, it resolves the problem of metal sintering deactivation caused by nickel core reaction and forms active phase nickel with small particle size and high dispersion. The methane conversion is high as 83%. In the second part, methane cracking reaction simulates high carbon deposition environment. Ni@CeO2-ZrO2 improved Ni@CeO2 deactivation, due to the poor thermal stability of CeO2 causes catalyst sintering and carbon deposition. Further, use CTAB as a porogen to improve catalyst catalytic ability. Ni@CeO2-ZrO2-1-0.5 is the best catalyst parameter, with nearly 60% methane conversion rate and no deactivation for 1 hour. The third part is the two-stage fluidized bed gasification waste PE catalytic hydrogen production experiment. We explore the effects of different catalyst structures on catalysis. Yolk shell structure catalyst is the most advantageous. Because of the hollow space between the core and shell may provide a homogenous for heterogeneous catalysis. The active phase core can sufficiently expose their active sites to enlarge the contact area with the reactants. The optimal hydrogen production is 730.6 mmol/h-g.

目錄
誌謝 i
摘要 ii
Abstract iii
目錄 v
圖目錄 viii
表目錄 xi
第一章 前言 1
1-1研究源起與動機 1
1-2研究目的 2
1-3 研究流程與架構 4
第二章 文獻回顧 6
2-1能源分布 6
2-1-1替代能源 7
2-1-2產氫來源 8
2-2廢棄物處理 17
2-2-1熱轉化處理技術 19
2-2-2塑膠氣化機制 21
2-2-3廢塑膠裂解-重組技術 22
2-3觸媒特性 26
2-3-1觸媒催化原理 26
2-3-2觸媒組成及種類 27
2-4負載型觸媒催化廢塑膠同時產氫產碳 28
2-5殼核型觸媒 31
2-6蛋黃型殼核觸媒 33
2-7功能性外殼 36
2-8文獻總結 39
第三章 實驗設備及方法 41
3-1實驗藥品及氣體 41
3-2實驗設備及分析儀器 42
3-3觸媒製備方法 43
3-3-1 活性相Ni核製備 43
3-3-2 Ni@SiO2殼核觸媒製備 44
3-3-3 Ni@CeO2蛋黃型殼核觸媒製備 44
3-3-4 Ni@CeO2-ZrO2蛋黃型殼核觸媒製備 45
3-3-5 Ni@CeO2-ZrO2殼核觸媒製備 47
3-3-6 Ni/CeO2-ZrO2負載型觸媒製備 48
3-4活性測試 49
3-5分析儀器之簡介 53
3-5-1穿透式電子顯微鏡(Transmission Electron Microscope, TEM)~ 53
3-5-2 X光粉末繞射儀(X-ray Power Diffraction, XRD) 54
3-5-3比表面積分析儀(Brunauer-Emmett-Teller, BET) 54
3-5-4 程序升溫還原系統 55
3-5-5 X射線光電子能譜儀(X-ray photoelectron spectroscopy, XPS) 55
3-5-6熱重分析儀(Thermogravimetric analyzer, TGA) 56
第四章 結果與討論 57
4-1 模擬廢塑膠氣化合成氣觸媒催化活性之評估 57
4-1-1 殼核結構對觸媒催化之影響 57
4-1-2 觸媒殼厚度及空間速度之影響 60
4-2甲烷裂解反應評估觸媒抗積碳能力 64
4-2-1鎳核及Ni@CeO2蛋黃殼核甲烷裂解反應活性測試 64
4-2-2 不同殼厚度之Ni@CeO2-ZrO2殼核觸媒甲烷裂解反應活性測試 65
4-2-3 Ni@CeO2-ZrO2添加開孔劑對觸媒催活性之影響 70
4-3二階段流體化床氣化廢PE催化產氫之測試 73
4-3-1不同觸媒結構之二階段流體化床氣化廢PE催化產氫活性測 73
第五章 結論與建議 79
5-1 結論 79
5-2建議 81
參考文獻 82

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