本研究針對木質纖維素、聚磷酸氨及碳奈米管等不同型態的環境友善補強材料或填充材，透過矽烷偶合劑、馬來酸酐或相容化劑等加以改質，並成功地與線性低密度聚乙烯及生物可分解脂肪族聚酯等環境相容材料加以複合，得到環境相容奈米複合材料。
本研究第一部份製備具水交聯反應之環境相容塑木複合材料。利用乙烯基偶合劑（VTMOS）做木質纖維素的偶合，先將具雙官能基的VTMOS之矽氧烷（-OCH3）端，與木質纖維的-OH基反應，VTMOS的另一端的乙烯基（-CH=CH2）則利用雙螺桿熔融反應押出時，以自由基反應方式接枝到基材（LLDPE、PBS）主鏈上，使其具有Sol-Gel的官能基，並藉由溫水進行水交聯反應。本系統所製備具水交聯反應之環境相容塑木複合材料，利用Solid State 13C-NMR證實，木質纖維素改質的VTMOS成功的接枝至PBS主鏈上，並且藉由1H-NMR圖譜下氫積分面積的比值，求得VTMOS接枝率為6.3%。複合材料的機械性質與熱性質，隨著水交聯時間的增加而增加。以具水交聯反應之木質纖維/LLDPE複合材料而言，當木質纖維含量為30wt%，且複合材料經4小時水交聯反應後，抗拉強度增加87%，抗折強度增加137.5%，而熱性質方面，熱變形溫度由55.7℃提升至88.5℃。
本研究第二部分製備APP/脂肪族聚酯生分解無鹵難燃複合材料。利用TEOS對APP進行偶合，並以熔融反應方式接枝到PBS主鏈上，藉由矽烷/水交聯的方式，一方面改善難燃劑APP與基材PBS之間的界面，藉以提昇複合材料的機械性質，另一方面藉由水交聯形成的網狀結構，改善基材燃燒時滴垂現象，使其達到阻燃的效果。結果發現，以TEOS含量1 phr改質之APP/PBS生分解難燃複合材料，以水交聯0.5小時後，交聯度達18.8%，所形成的Si-O-Si網狀結構能有效抑制滴垂效應，使UL-94 達V0等級，而以水交聯4小時後，L.O.I值更達到28（提升16.7%）可有效降低APP難燃劑的添加量。
本研究第三部份製備具水交聯反應碳奈米管/線性低密度聚乙烯奈米複合材料。首先將乙烯基矽烷偶合劑（VTMOS）接枝到LLDPE基材上，同時多壁碳奈米管（MWNT）利用自由基的方式，將VTMOS接枝到MWNT上（VTMOS-g-MWNT），形成碳奈米管及基材上均具有可進行Sol-Gel水交聯的官能基，然後將此二者以雙螺桿熔融混摻（System 2）。另外，也比較MWNT以VTMOS偶合處理，再進行雙螺桿熔融反應押出的方式（System 1）。僅添加0.5 phr 含量的VTMOS-g-MWNT /LLDPE奈米複合材料，可有效提升基材的拉伸強度65.6%，及衝擊強度24.8%，基材經4小時水交聯反應之後，熱變形溫度大幅提昇32.8%，熱裂解溫度提升42℃。
本研究第四部份製備的具導電性質碳奈米管/聚乳酸奈米複合材料。利用自由基反應的方式，將具有碳碳雙鍵的馬來酸酐接枝到多壁碳奈米管上，以提供MWNT與基材PLA之間，產生化學鍵結及物理鍵結，而增加兩材質之間的界面相容性。並探討多壁碳奈米管（MWNT）添加於高結晶性PLA（high-crystalline PLA, HC-PLA）與低結晶性PLA（low-crystalline PLA, LC-PLA），比較結晶性的高低對於導電奈米生物可分解複合材料的電氣性質、機械性質、熱性質的影響。添加碳奈米管可有效提升PLA基材的機械強度及熱性質。且電氣性質方面，未改質碳管與改質碳管含量為0.5 phr時，基材的表面電阻即產生大幅的變化；當同樣含量未改質碳管補強的基材之表面電阻於LC-PLA（2.8×109 Ω/□）中，遠低於HC-PLA（1.05×1013 Ω/□）。而改質的碳奈米管當含量0.5 phr時，在LC-PLA基材的表面電阻比純LC-PLA下降了1013 orders（5.46×1015 至 2.61 × 102 Ω/□）。碳奈米管可誘導低結晶性聚乳酸產生結晶，此現象可藉由MA改質的MA-g-MWNT，在基材中的分散程度所控制。

This research utilized different environmental friendly reinforcements or fillers, such as cellulose, ammonium polyphosphate, and carbon nanotube, to reinforce the environmentally conscious polymer, such as linear low-density polyethylene and biodegradable polyester, forming the eco- and nano-composites.
Wood flour (WF) reinforced linear low-density polyethylene (LLDPE) composites were prepared in the first part of this dissertation. Water-crosslinking technique was used to improve the physical properties of wood composite. Composites were compounded in a twin-screw extruder and treated with a coupling agent (vinyltrimethoxysilane, VTMOS), and then moisture-crosslinked in hot water. Composite after water-crosslinking treatment exhibited better mechanical properties than the non-crosslinked one because of the improved chemical bonding between the wood fiber and the polyolefin matrix. As the wood flour content reaches to 30wt% and after water-crosslinking for 4 hours, tensile strength and flexural strength are increased by 87%（from 14.7 to 27.5 MPa）and 137.5％（from 11.2 to 26.6 MPa）with respect to that of non-crosslinked ones. Photographs of Scanning Electron Microscopy (SEM) of the fracture surfaces of water-crosslinked composites showed superior interfacial strength existed between the wood fiber and the polyolefin matrix. Thermal analyses of water-crosslinked composites indicate that thermal degradation temperature and heat deflection temperature of composite increase with the increasing of water-crosslinking time. The heat deflection temperature of the composite can be raised from 55.7□C to 88.5□C.

The preparation and characterization on the novel water-crosslinked cellulose reinforced poly (butylene succinate) composites have been conducted. Wood flour (raw cellulose) reinforced poly (butylene succinate) (PBS) composites have been prepared utilizing unique water-crosslinking technique to improve the physical properties of composites. The composites were treated with a coupling agent ( Vinyltrimethoxysilane ) and then were compounded in a twin screw extruder. The compound was moisture-crosslinked. 13C NMR, 1H NMR and FT-IR spectra were utilized to monitor and characterize the water-crosslinking reaction. Composites via water-crosslinking treatment exhibits improved mechanical properties due to the interfacial bonding between the wood fiber and the PBS matrix. SEM microphotographs of the fracture surfaces of water-crosslinked composites showed superior interfacial linkage existed between the wood fiber and the PBS matrix. Thermal analysis on the water-crosslinked composites indicated that thermal degradation temperature of composite increased with the increasing of water-crosslinking time. POM microphotographs revealed that the water-crosslinking reaction can increase the crystalline rate but decrease the spherulites size of PBS. Biodegradation tests showed that adding wood flour increased the biodegradability of composite; however, the water-crosslinking reaction may reduce the biodegradability of wood composite.

The second part of this dissertation focuses on the effect of water-crosslinking reaction on the flame retardancy and non-dripping properties of ammonium polyphosphate / poly (butylene succinate) composites. Ammonium polyphosphate (APP) reinforced poly (butylene succinate) (PBS) composites have been prepared utilizing a unique water-crosslinking technique to improve the flame retardancy and non-dripping property of composites, meanwhile, maintain the main structure of composites. The composites were treated with a coupling agent ( Tetraethoxysilane, TEOS ) and then were compounded in a twin screw extruder. The compound was moisture-crosslinked. FT-IR spectra were used to monitor the water-crosslinking reaction. Composites via water-crosslinking treatment exhibits improved mechanical properties due to the interfacial bonding between the APP and the PBS matrix. Microphotographs of SEM of the fracture surfaces of water-crosslinked composites showed the void size was increased with the increasing of water-crosslinking time. Composite with 15wt% APP were classified as UL-94 V-2. However, the ones with only 0.5 hr water-crosslinking reaction were classified as UL-94 V-0. Thermal analysis on the water-crosslinked composites indicated that thermal degradation temperature of composite increased with the increasing of water-crosslinking time. DSC results revealed that the water-crosslinking reaction can limit the crystalline rate of PBS.

The third part of this dissertation is the preparation of carbon nanotube / linear low density polyethylene composites by a water-crosslinking reaction. A novel method to prepare the multiwall carbon nanotube (MWCNT) / linear low density polyethylene composite is demonstrated. The combination of free radical reaction and water-crosslinking reaction to prepare the MWCNT/LLDPE composite was characterized by Raman and FT-IR. Mechanical properties and thermal stability of composite were significantly improved after silane modification and water-crosslinking reaction. The crosslinking network between LLDPE and carbon nanotube plays a vital role for the improvement of mechanical properties and thermal stability of composite. The tensile strength and impact strength of 0.5 phr VTMOS-g-MWCNT / LLDPE composites can increase 65.6% and 24.8%, respectively, comparing with pristine MWCNT /LLDPE composites. The heat deflection temperature of 4phr VTMOS-g-MWCNT / LLDPE composites (via 4 hr water-crosslinking reaction) was 79.7□C, which is much higher than pristine LLDPE (60.0□C). Thermal degradation temperature of composite can increase 42oC via silane modification and water-crosslinking reaction.

The fourth part of this dissertation is to elucidate the mechanical, electrical and thermal characteristics of novel multi-wall carbon nanotubes / lowly and highly crystalline poly (lactic acid) nanocomposites. This work presents a new approach to prepare multi-wall carbon nanotubes / polylactide (PLA) nanocomposite. Comparisons of carbon nanotube-reinforced high-crystalline and low-crystalline PLA nanocomposites were discussed. High electrical conductivity of nanocomposite can be achieved at a low carbon nanotube loading. When only 0.5phr modified MWNT was added to LC-PLA, the surface resistance of the nanocomposite reduced from 5.46×1015 to 2.61 × 102 Ω/□ (by 1013 orders). Carbon nanotubes cause the mechanical characteristics of low-crystalline PLA to be better than those in high-crystalline PLA. Only 0.5 phr modified MWCNT induces crystallization, and improves the thermal properties of the nanocomposite. The extent of the dispersion of carbon nanotubes in low-crystalline PLA matrix can be used to control carbon nanotube-induced crystallization

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