耐熱型聚乳酸與非耐熱型聚乳酸塑膠回收再利用過程之特性研究

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潘冠蓁(Quan-Jhen Pan) 查詢紙本館藏

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耐熱型聚乳酸與非耐熱型聚乳酸塑膠回收再利用過程之特性研究
(Characteristics Study of Recycling Process for Polylactic Acid (PLA) and Crystalline Polylactic Acid (CPLA))

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至系統瀏覽論文 (2028-1-1以後開放)

摘要(中)

1980年代，台灣環保意識抬頭，從1950年代以來普遍被使用的塑膠，也因為其原料來自於有限的石油，製造時不僅會造成環境汙染，使用後又不易分解，塑膠製品已經廣泛使用多年，但在一次性使用後所拋棄的塑膠廢棄物引發的環境議題受各國廣泛關注，進而熱議討論及尋找取代方案，而聚乳酸塑膠(Polylactic Acid, 以下簡稱為PLA)成為許多塑膠產品的替代方案，因為當聚乳酸塑膠在適當溫度及濕度的堆肥環境時，會被微生物快速地分解，若是試算全球的塑膠預計使用量，仍然需要大面積的土地作為堆肥使用。而本研究主要是探討非耐熱型聚乳酸(PLA)以及耐熱型聚乳酸(Crystalline Polylactic Acid, 以下簡稱為CPLA)之比較，可生物分解之塑膠製品回收再利用的可行性，回收過程中分子量降解的過程比較，在不同的氫氧化鈉清洗濃度和不同清洗溫度的條件下，進行聚乳酸生物可分解塑膠之物化性質以及熱性質的分析比較。
本研究為了解PLA和CPLA塑膠回收再利用之可行性探討，採用美國材料暨試驗協會(American Society for Testing and Materials, ASTM) G154 Cycle A的標準方法作為老化條件，此方法是最廣為使用的加速老化試驗之一，模擬陽光、溫度對塑膠材料的破壞作用，其塑膠材料老化包含強度降低、褪色、龜裂、脫落、粉化和氧化等等，樣品在模擬的環境中從幾個小時甚至數天的時間，可體現在戶外幾個月或是數年發生的損害。本研究將分成無照光老化條件的聚乳酸塑膠分解情形比較，以及使用UVA-340燈管照射8小時後，接著進入4小時黑暗期，總共循環20次，(總)實驗時長為240小時，其老化的加速倍數約為12倍，將探討有無經過照光老化240小時之PLA和CPLA進行熱性質與物化性質分析。

摘要(英)

Environmental issues caused by single-use plastic products have received extensive attention from various countries, and have been banned and replaced. Polylactic acid plastic has become an alternative for many products to be used. PLA plastics are rapidly decomposed by microorganisms in a compost field with appropriate temperature and humidity, but compared with the global usage, a large area of land is still required for composting. The purpose of this study is to investigate the aging of PLA plastics in 10 days, the comparison of molecular degradation during the recovery process, the analysis and comparison of the physical and chemical properties of the recovered PLA w carried out at higher NaOH concentration and higher cleaning temperature.
To understand the aging of polylactic acid wastes exposed to environmental, the accelerated aging standard method of American Society for Testing and Materials (ASTM) G154 was used, and polylactic acid fragments were exposed to air. Then, put it into the weather resistance testing machine (UVA lamp), the accelerated aging rate of this condition is about 12 times, and in order to understand the effect of light on the aging reaction, no light is used as the control group, both groups were aged for 10 days for physical property analysis.

關鍵字(中)

★ 聚乳酸
★ 老化
★ 生物可分解

關鍵字(英)

★ PLA
★ Aging
★ Biodegradable

論文目次

目錄
摘要 I
Abstract II
目錄 IV
圖目錄 VII
表目錄 IX
第一章前言 1
1.1 研究緣起 1
1.2 研究目標 2
1.3 研究特色 2
第二章文獻回顧 4
2.1 塑膠歷史與應用 4
2.2 聚乳酸塑膠(PLA) 7
2.2.1 直接縮聚法(Condensation Polymerization) 11
2.2.2 開環聚合法(Ring-Opening Polymerization) 13
2.3 耐熱型聚乳酸塑膠(CPLA) 15
2.3.1 PLA結晶性質介紹 15
2.3.2 PLA奈米複合材料 16
2.3.3 PLA混摻多種複合材 17
2.4 PLA分解機制 18
2.5 PLA光解機制 20
2.6 PLA塑膠回收 21
2.6.1 水解法 22
2.6.2 熱解法 23
2.6.3 醇解法 23
2.6.4 醣解法 24
2.6.5 氨解法 24
第三章實驗方法 25
3.1 研究架構與規劃 25
3.2 實驗方法與步驟 27
3.2.1 PLA與CPLA來源 27
3.2.2 模擬老化試驗 28
3.2.3 實驗製備步驟 29
3.3 實驗儀器設備 30
3.3.1 耐候試驗機(Weather-Proofing Tester) 30
3.3.2 衰減全反射傅立葉紅外線光譜儀(Attenuated Total Reflection - Fourier Transform Infrared Spectroscopy, ATR-FTIR) 31
3.3.3 差示熱掃描分析儀(Differential Scanning Calorimetry，DSC) 32
3.3.4 X-光繞射分析儀(X-ray diffractometer, XRD) 33
3.3.5 熱重量分析儀(Thermogravimetric Analysis, TGA) 34
3.3.6 特性黏度計(Inherent Viscosity，IV) 35
3.3.7 掃描式電子顯微鏡(Scanning Electron Microscope, SEM) 36
3.4 實驗藥品 37
第四章結果與討論 38
4.1 IV特性黏度分析 38
4.1.1 分子量比較 38
4.1.2 不同清洗溫度 49
4.1.3 不同清洗濃度 50
4.1.4 不同清洗時間 52
4.1.5 有無照光老化 53
4.2 DSC分析 55
4.3 TGA分析 62
4.4 FTIR分析 69
4.5 XRD分析 71
4.6 SEM分析 73
第五章結論與建議 76
5.1 結論 76
5.2 建議 78
參考文獻 79
附錄 89
附錄一學位考試委員意見回覆表 89

圖目錄
圖 1從農產品生產PLA的製作過程 6
圖 2熱塑性與熱固性分子結構圖 8
圖 3 D-型與L-型聚乳酸單體結構圖 9
圖 4 環狀丙交酯結構式 10
圖 5 直接縮聚法示意圖 11
圖 6 聚合期間PLA所發生的反應 11
圖 7 乳酸聚合成PLA流程圖 12
圖 8 聚乳酸開環聚合法流程圖 14
圖 9 PLA降解反應過程 19
圖 10 PLA回收路徑圖 21
圖 11 從葡萄糖發酵和PLA熱解聚反應生產乳酸所需負荷總能量 23
圖 12 研究架構圖 26
圖 13 市售商業用 (a) PLA塑膠杯 (b) CPLA杯蓋 27
圖 14 模擬老化耐候試驗機 28
圖 15 FTIR-ATR光譜設置 31
圖 16 X-光繞射分析儀 34
圖 17黏度管(Ubbelohde Viscometers) 36
圖 18 掃描式電子顯微鏡分析原理圖 37
圖 19 不同溫度PLA分子量比較 49
圖 20 不同清洗溫度CPLA分子量比較 50
圖 21 不同清洗濃度的PLA分子量比較 51
圖 22 不同清洗濃度的CPLA分子量比較 51
圖 23不同清洗時間PLA分子量比較 52
圖 24 不同清洗時間CPLA分子量比較 52
圖 25不同條件清洗(a)未照光老化PLA以及(b)有照光老化PLA 54
圖 26 照光老化PLA在90℃的10% NaOH溶液中清洗90分鐘 54
圖 27不同條件清洗(a)未照光老化CPLA以及(b)有照光老化CPLA 54
圖 28 照光老化CPLA在90℃的10% NaOH溶液中清洗90分鐘 54
圖 29 原樣PLA之DSC圖譜 56
圖 30 有照光老化240小時環境下PLA之DSC圖譜 56
圖 31 無照光老化CPLA之DSC圖譜 60
圖 32 有照光老化240小時環境下CPLA之DSC圖譜 60
圖 33 Virgin PLA與Aging PLA以及鹼洗PLA熱重(TG)曲線圖 63
圖 34 Virgin PLA與Aging PLA以及鹼洗PLA熱重微分(DTG)曲線圖 63
圖 35 Virgin CPLA與Aging CPLA以及鹼洗CPLA熱重(TG)曲線圖 67
圖 36 Virgin CPLA與Aging CPLA以及鹼洗CPLA熱重微分(DTG)曲線圖 67
圖 37 有無照光老化與鹼洗(a) PLA和(b) CPLA之FTIR分析 70
圖 38 原樣CPLA與高溫鹼洗後CPLA之XRD圖譜 72
圖 39 原樣CPLA與高溫鹼洗後CPLA之XRD疊圖比較 72
圖 40 (a)原樣PLA、(b)照光老化PLA、(c)與(d)鹼洗PLA之SEM比較圖 73
圖 41 鹼洗Aging PLA之SEM比較圖 74
圖 42 (a)原樣CPLA與(b)照光老化CPLA之SEM比較圖 74
圖 43 (a)照光老化CPLA與(b)鹼洗CPLA之SEM比較圖 75
圖 44照光老化240小時後鹼洗CPLA之SEM比較圖 75

表目錄
表 1目前開發之綠色塑膠 5
表2 實驗藥品清單 37
表 3 無照光老化PLA分子量 40
表 4 有照光老化240小時PLA分子量 42
表 5 無照光老化CPLA分子量 45
表 6 有照光老化240小時CPLA分子量 47
表 7 原樣PLA與有照光老化240小時PLA之DSC熱性質比較 58
表 8 原樣PLA與有照光老化240小時CPLA之DSC熱性質比較 61
表 9 Virgin PLA與Aging PLA熱性質TGA比較 65
表 10 Virgin CPLA與Aging CPLA熱性質TGA比較 68

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指導教授

林伯勳(Po-Hsun Lin)

審核日期

2024-5-1

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