TWI778957B - 包含聚（甲基）丙烯醯亞胺發泡體粒子的聚合物混合物 - Google Patents
包含聚（甲基）丙烯醯亞胺發泡體粒子的聚合物混合物 Download PDFInfo
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Abstract
該本發明關於一種聚合物混合物，其包含熱塑性樹脂及聚(甲基)丙烯醯亞胺(P(M)I)發泡體粒子。該本發明之聚合物混合物達成比個別組分較佳之機械性能，且可廣泛用於輕量構造物中。
Description
本發明關於一種聚合物混合物，其包含聚(甲基)丙烯醯亞胺(P(M)I)發泡體粒子，尤其是聚甲基丙烯醯亞胺(PMI)發泡體粒子。
聚(甲基)丙烯醯亞胺發泡體，例如聚甲基丙烯醯亞胺發泡體，諸如由Evonik Resource Efficiency GMBH所行銷之商標為Rohacell®者，由於其輕量及高機械性能，故廣泛用於輕量設計所需之複合材料中，以供用於航太、車輛、運動及醫藥裝置工業等。
以前P(M)I發泡體係以塊狀供應，然而其不完全適合具有複雜三維幾何形狀之部件的加工，且可能會導致長的循環時間、低的精確度、及材料之浪費。
WO 2013/056947敘述一種P(M)I發泡體之模製成型方法，其部分解決了以上難題，其中(預發泡之)P(M)I聚合物粒子於模中藉黏合劑之助而發泡，該黏合
劑可為聚醯胺或聚(甲基)丙烯酸酯。該黏合劑之劑量可為高至P(M)I聚合物粒子之20%，亦即以P(M)I聚合物粒子與黏合劑之總重量為基準為高至16.7%。然而此方法仍導致長的循環時間。
為了解決上述難題，本案發明人探索P(M)I發泡體粒子與熱塑性樹脂形成聚合物混合物之可能性，因而完成本發明。
本發明提供一種聚合物混合物，其包含：(1)熱塑性樹脂，其於低於400℃之溫度下為可熔融加工的，及(2)聚(甲基)丙烯醯亞胺發泡體粒子，其於低於400℃之溫度下保持為粒狀形式，其中，以該聚合物混合物之總重量為基準，該熱塑性樹脂占20-99%，且該P(M)I發泡體粒子占1-80%。
令人驚訝地發現，本發明之聚合物混合物除了輕量之外，還達成比個別組分較佳之抗壓及/或抗彎強度。
本發明還提供一種製造本發明之聚合物混合物之方法，其包括物理性混合該聚(甲基)丙烯醯亞胺發泡體粒子與該熱塑性樹脂之熔融體之步驟。
本發明還提供本發明之該聚合物混合物用於輕量構造物中之用途。
對於該熱塑性樹脂並無限制，只要其於低於400℃之溫度下為可熔融加工的即可。可熔融加工在此係依其習用意義應用，亦即該聚合物可在所指定之溫度下加工而無聚合物之實質降解。
該熱塑性樹脂之實例包括聚醯胺、聚烯烴、聚酯及包含任何該以上片段之共聚物以及它們的摻合物。
較佳的是，該聚醯胺為選自脂族聚醯胺，更佳為選自PA6、PA11、PA12、PA46、PA66、PA10、PA610、PA612、PA1010、PA1012及它們的摻合物。
用於本發明中之P(M)I發泡體粒子，可經由不為粒狀形式之P(M)I發泡體之粒化作用而獲得。
該P(M)I發泡體亦稱為剛性發泡體，且其特徵為具有特別之韌性。該P(M)I發泡體通常以二階段方法製造：a)製造鑄型用聚合物，及b)發泡該鑄型用聚合物。然後依照先前技術，將彼等切割或鋸成所需之形狀。
該P(M)I發泡體之製造起始於單體混合物之製造，該單體混合物包含作為主要組分之(甲基)丙烯酸及(甲基)丙烯腈，其莫耳比較佳為2：3至3：2。亦可使用其他共聚單體，實例為丙烯酸或甲基丙烯酸之酯、苯乙烯、順丁烯二酸及亞甲基丁二酸及其酐，以及乙烯基吡咯啶酮。
然而，該等共單體之比例在此應不高於30重量%。亦可使用少量之交聯單體，實例為丙烯酸烯丙酯。然而，其量較佳應為至多0.05重量%至2.0重量%。
共聚合作用之混合物還包含發泡劑，其於150至250℃之溫度下會分解或蒸發，且因此形成一氣相。聚合作用於低於此溫度下進行，該鑄型用聚合物因此包含一潛在之發泡劑。該聚合作用係有利地在二玻璃板之間的塊形模中進行。
該鑄型用聚合物然後於第二步驟中在適當之溫度下發泡。此種P(M)I發泡體之製造原則上為熟習此技術之人士已知的，且例如可見於EP 1 444 293、EP 1 678 244或WO 2011/138060中。
用於本發明中之P(M)I發泡體粒子亦可經由發泡P(M)I聚合物粒子而獲得。
該P(M)I聚合物粒子可經由例如於切割式粉碎機中研磨該鑄型用聚合物而獲得。然後將該研磨體在適當溫度下發泡而製造P(M)I發泡體粒子。
用於本發明中之該P(M)I發泡體粒子較佳為經由發泡P(M)I聚合物粒子而獲得，其與經由P(M)I發泡體之粒化作用所獲得之P(M)I發泡體粒子相比，封閉之發泡體小室不會被破壞。
該P(M)I發泡體粒子較佳具有範圍在0.1-30毫米，更佳為0.5-10毫米之粒徑。
該P(M)I發泡體粒子較佳具有25-220kg/m3，
更佳為50-150kg/m3之體密度。
於本發明之一較佳實施體系中，該P(M)I發泡體粒子為聚甲基丙烯醯亞胺(PMI)發泡體粒子。
尤其可提到的是來自Evonik Resource Efficiency GMBH之市售Rohacell® PMI聚合物及/或發泡體。
於本發明之聚合物混合物中，該熱塑性樹脂及該P(M)I發泡體粒子之比例並無限制。
以該聚合物混合物之總重量為基準，該熱塑性樹脂可占20-95%，較佳為20-80%，更佳為30-70%，且該P(M)I發泡體粒子可占5-80%，較佳為20-80%，更佳為30-70%。但以該聚合物混合物之總重量為基準，亦可為該熱塑性樹脂占1-99%，且該P(M)I發泡體粒子可占1-99%。
於本發明之一較佳實施體系中，該熱塑性樹脂於低於250℃之溫度下為可熔融加工的，及/或該P(M)I發泡體粒子於低於250℃之溫度下保持為粒狀形式。
本發明之聚合物混合物可包括添加物，例如碳酸鈣、玻璃珠、氧化鋅、及纖維強化體諸如陶瓷纖維、聚芳醯胺纖維、鈦酸鉀纖維、玻璃纖維及碳纖維，視所需之功效或性能而定。
本發明之聚合物混合物原則上一般為適用於任何類型之輕量構造物，且尤其可用於例如大量製造汽車
工業中之車身構造物或內部包覆物、軌道車輛構造或造船工業中之內部部件、航太工業、機械工程、運動設備之製造、傢俱建造或風力渦輪發電機之設計。
由以商標ROHACELL® Triple F而為Evonik Resource Efficiency GMBH所行銷之PMI聚合物粒子製備實施例中使用之PMI發泡體粒子。該PMI聚合物粒子係由經完全聚合之共聚物片(其未經預發泡)藉造粒機之助而製造。用於實施例之粒子於過篩以保留細小粒子後，其粒徑範圍為低於1.0毫米。該PMI聚合物粒子之體密度為約600-700kg/m3。
該PMI聚合物粒子係於烤箱中在200-240℃之溫度下發泡30-60分鐘。所獲得之PMI發泡體粒子具有100-150kg/m3之體密度及0.5-5毫米之粒徑。
將該PM.I發泡體粒子分別與PA12(Evonik Resource Efficiency GMBH所製之Vestamid® L1600)及PA12彈性體(Evonik Resource Efficiency GMBH所製之Vestamid® E30，聚醚嵌段PA12)之熔融體混合，而製備兩種50：50(重量)混合物，它們經成型為具有5毫米厚度之板。
測試該等板之抗壓強度(ISO 844)及抗彎強度(ISO 178)以及密度。結果示於下表中。
由以上可看出對於Vestamid LI600及Vestamid E30二者皆達成高於25%之重量減低。而且該等實施例之聚合物混合物達成比個別原料較高之抗壓及/或抗彎強度。
Claims (11)
- 一種聚合物混合物，其包含：(1)熱塑性樹脂，其於低於400℃之溫度下為可熔融加工的，及(2)聚(甲基)丙烯醯亞胺(P(M)I)發泡體粒子，其於低於400℃之溫度下保持為粒狀形式，其中，以該聚合物混合物之總重量為基準，該熱塑性樹脂占30-70%，且該P(M)I發泡體粒子占30-70%，其中該P(M)I發泡體粒子具有範圍在0.1-30毫米之粒徑，及其中該P(M)I發泡體粒子具有25-220kg/m3之體密度。
- 如申請專利範圍第1項之聚合物混合物，其中該熱塑性樹脂為選自聚醯胺、聚烯烴、聚酯及包含任何以上片段之共聚物以及它們的摻合物。
- 如申請專利範圍第2項之聚合物混合物，其中該聚醯胺為選自脂族聚醯胺。
- 如申請專利範圍第2項之聚合物混合物，其中該聚醯胺為選自下列所組成之群組：PA6、PA11、PA12、 PA46、PA66、PA10、PA610、PA612、PA1010、PA1012及它們的摻合物。
- 如申請專利範圍第1-4項中任一項之聚合物混合物，其中該P(M)I發泡體粒子具有範圍在0.5-10毫米之粒徑。
- 如申請專利範圍第1-4項中任一項之聚合物混合物，其中該P(M)I發泡體粒子具有50-150kg/m3之體密度。
- 如申請專利範圍第1-4項中任一項之聚合物混合物，其中該P(M)I發泡體粒子係經由下述方式獲得：(1)不為粒狀之P(M)I發泡體之粒化作用，或(2)發泡P(M)I聚合物粒子。
- 如申請專利範圍第1-4項中任一項之聚合物混合物，其中該P(M)I發泡體粒子為聚甲基丙烯醯亞胺(PMI)發泡體粒子。
- 如申請專利範圍第1-4項中任一項之聚合物混合物，其中該熱塑性樹脂於低於約250℃之溫度下為可熔融加工的，及/或該P(M)I發泡體粒子於低於250℃之溫度下保持為粒狀形式。
- 一種製造如申請專利範圍第1-9項中任一項之聚合物混合物之方法，其包括物理性混合該P(M)I發泡體粒子與該熱塑性樹脂之熔融體的步驟。
- 一種如申請專利範圍第1-9項中任一項之聚合物混合物之用途，其係用於輕量構造物。
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| EP4200111B1 (de) | 2020-08-18 | 2024-09-04 | Evonik Operations GmbH | Herstellung von granulaten auf basis von hochtemperatur-polymeren mittels unterwassergranulierung bei erhöhter wassertemperatur |
| EP4469507A1 (en) | 2022-01-24 | 2024-12-04 | Röhm GmbH | Polymer foams based on blends of poly(vinylidene fluoride) and poly(meth)acrylimide |
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| DE10141757A1 (de) * | 2001-08-29 | 2003-03-27 | Roehm Gmbh | Verbessertes Verfahren zur Herstellung von PMI-Schäumen |
| EP1914052B1 (de) * | 2006-10-19 | 2017-06-28 | Basf Se | Leichte Holzwerkstoffe |
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| CN101857656B (zh) * | 2010-05-24 | 2011-08-31 | 四川大学 | 用于生产聚甲基丙烯酰亚胺泡沫材料的可发性颗粒及应用 |
| JP5814551B2 (ja) * | 2011-01-19 | 2015-11-17 | 積水化学工業株式会社 | 発泡成形体 |
| DE102012208428A1 (de) * | 2012-05-21 | 2013-11-21 | Evonik Industries Ag | Pul-Core-Verfahren mit PMI-Schaumkern |
| DE102013223347A1 (de) * | 2013-11-15 | 2015-05-21 | Evonik Industries Ag | Mit Poly(meth)acrylimid-Schaum gefüllte Wabenstrukturen |
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| WO2017167197A1 (en) | 2017-10-05 |
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