TW201532826A - 包含聚(甲基)丙烯酸醯亞胺泡沫體之蜂巢結構 - Google Patents
包含聚(甲基)丙烯酸醯亞胺泡沫體之蜂巢結構 Download PDFInfo
- Publication number
- TW201532826A TW201532826A TW103139222A TW103139222A TW201532826A TW 201532826 A TW201532826 A TW 201532826A TW 103139222 A TW103139222 A TW 103139222A TW 103139222 A TW103139222 A TW 103139222A TW 201532826 A TW201532826 A TW 201532826A
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- Prior art keywords
- honeycomb
- foam
- particles
- structural material
- lightweight structural
- Prior art date
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Abstract
本發明關於一種包含聚(甲基)丙烯酸醯亞胺(P(M)I)泡沫體之蜂巢結構之製法。在此方法中將較佳能已經預發泡之P(M)I粒子填入蜂巢結構之個別蜂巢,且接著進行熱發泡反應。
同時,本發明也包含藉由前述方法所製造之新穎材料,該材料具有極低重量且結合該蜂巢結構之諸多優點(例如高垂直強度和耐衝擊性)與該P(M)I泡沫體之諸多優點(特別是於所有方向之高壓縮強度及高韌性)。
Description
在輕質結構(特別是航空結構)之領域中,而且在汽車結構中也逐漸地,有兩種類型之擔負重量節省結合高強度之前導位置的技術:蜂巢結構及剛性泡沫體材料。
本發明關於一種包含聚(甲基)丙烯酸醯亞胺(P(M)I)泡沫體之蜂巢結構之製法。在此方法中將較佳能已經預發泡之P(M)I粒子填入蜂巢結構之個別蜂巢,且接著進行熱發泡反應。
同時,本發明也包含藉由前述方法所製造之新穎材料,該材料具有極低重量且結合該蜂巢結構之諸多優點(例如高垂直強度和耐衝擊性)與該P(M)I泡沫體之諸多優點(特別是於所有方向之高壓縮強度及高韌性)。
在輕質結構中蜂巢結構(特別是由金屬如鋁、鈦或鋼製造)有長久之歷史。這些結構不僅有輕質,還有非常好之垂直強度的主要優點。該簡稱蜂巢有時候也用於這些蜂巢結構。在上下文中“垂直”意指“依開式蜂巢之方向”。當
適當表面已經由某材料如金屬板材或木板,或由複合材料,覆蓋時前述強度特別是非常高。然而,這些結構之缺點是就側壓來看極其不穩定。
再者,當應用以樹脂為底質之複合材料的形式之外層時金屬蜂巢的缺點是這些難以依樹脂灌注法(resin infusion process)處理,因為由於成本和重量的緣故,樹脂無法完全填滿個別單元。相對於以下隨後階段所述之剛性泡沫體,此處需要的是複雜之事前密封方法。
該蜂巢結構之其他缺點是斜面蜂巢邊緣必需填充,因為該蜂巢具有一點點吸收側向力之能力,且未完全密封之蜂巢易受凝結水進入所影響。即使僅因為伴隨而來之重量增加,後者卻是尤其是在飛行時之主要問題。
除了前述金屬蜂巢之外的選擇是剛性泡沫體,特別是由聚甲基丙烯醯胺(PMI)或聚甲基丙烯醯亞胺(PI)-這些之簡寫講法是聚(甲基)丙烯酸醯亞胺(P(M)I)。剛性泡沫體能以輕質結構按板產物使用。關此,藉著與該蜂巢類似,上側和任意地下側係以金屬板材或木板或以複合板當外層覆蓋。該覆蓋物對該剛性泡沫體之接合,之後將其稱為泡沫芯體或芯材,一般係藉由黏著接合或拼接(stitching)或藉由插銷接合達成。此類型拼接方法係藉由EP 2 203 298之實施例描述。藉由插銷將外層接合於泡沫芯體係由EP 1 907 193之實施例見到。
然而,剛性泡沫體材料之缺點是其並非耐衝擊性。儘管這能藉由引進外層抵銷,但是卻多半無法防禦側面效
應。再者這也是改善關於外層之垂直強度的穩定性的必備條件,不僅是在蜂巢芯體之案例,在剛性泡沫芯體之案例也一樣。
DE 18 17 156和DE 27 26 260描述即使是於高溫也具有優良機械性質之PMI泡沫體的製法。該泡沫體係藉由鑄造法製造,即單體和其他必要物質係於艙中混合並聚合。在第二步驟時,該聚合物係藉由加熱發泡。除了這些PMI泡沫體之外,也知道有以具有類似性質之甲基丙烯酸和丙烯腈為底質之泡沫體(PI泡沫體)。這些係藉由CN 100420702C之實施例描述。這些泡沫體最初也製造成板。
除了從沒發泡之聚合物板開始的這些方法之外,也有從細粒開始之所謂的模具內發泡法(in-mould foaming process)。然而,當這些與所述之方法相比時,其具有許多根本之缺點。達成的是不均一之細孔結構,其原始粒子之內部與原始粒子間之邊界之間有差異。再者,由於發泡程序時之粒子不均勻分佈-如前所述,使該泡沫體之密度也不均勻。在這些產物上可能觀察到的是在該發泡程序時原始粒子間形成之邊界處的凝聚力較不足,及與板產物半成品所發泡之材料相比所得之機械性質較不足。
WO 2013/05947描述一種模具內方法,其中至少後面之問題已經藉由在填入用於發泡程序之成形模具之前給粒子塗佈黏著促進劑,例如聚醯胺或聚甲基丙烯酸酯,而獲得解決。因此達成於該晶粒邊界處之非常好的黏著力。然
而,此方法卻未消除最終產物之不均勻細孔分佈。
有鑑於討論過之先前技藝,因此本發明之目的在於提供具有忍受特高機械負荷之能力的新穎輕質結構材料,其特別是能用作供輕質結構用之複合夾層材料的芯材。在此機械強度不僅包含高耐衝擊性,還有高壓縮強度。
特別是,本發明之一目的在於提供新穎之複合材料,當其兩側係鋪以外層且因此採行夾層材料之形式時,其相對於前述外層之垂直方向具有比先前技藝好之壓壓縮強度。
再者,當這些複合材料係暴露於側向效應(lateral effect)時,即直接作用於該芯材之效應,吾人不僅意欲其具有比剛性泡沫芯體好之耐衝擊性,還有比金屬蜂巢芯體好之壓壓縮強度。
再者吾人意欲的是能快速且輕易地進行前述輕質結構材料(特別是依夾層材料之形式)之製法。
再者,吾人意欲該芯材易於進行容易之進一步加工,例如藉由用於製造外層之樹脂澆注法或注入法。
還有其他此處未曾清晰討論之目的能從先前技藝、說明書、申請專利範圍或實施態樣推衍出來。
當後文中使用該措辭聚(甲基)丙烯酸醯亞胺(P(M)I)
時,其意指聚甲基丙烯醯胺(PMI)、聚甲基丙烯醯亞胺(PI)或其混合物。類似之考量適於相應之單體如(甲基)丙烯醯亞胺和(甲基)丙烯酸。舉例來說,該措辭(甲基)丙烯酸不僅意指甲基丙烯酸,還有丙烯酸或二者之混合物。
該目的係藉由提供一種包括含P(M)I之蜂巢的輕質結構材料達成。
特別是,前述輕質結構材料之設計可以使該包含P(M)I泡沫體之蜂巢採芯材板形式,且前述芯材於一或二側具有外層。
該外層較佳為金屬板材或木板或複合板,藉由拼接或黏著接合或藉由針腳接合於該芯材。在此特別適合之金屬係鋁、鎂、鋼和鈦。
驚人的是,該外部材料可相對任意地選用。在此複合材料舉例來說可簡單地包含熱塑性塑膠或編織物或針織物或其複合材料,例如所謂之有機嵌板或塗佈塑料之紡織承載布,例如合成皮革。較佳為該外部材料係纖維補強塑膠。該纖維可接著舉例來說為聚芳醯胺纖維(aramid fibre)、玻璃纖維、碳纖維聚合物纖維或紡織纖維。該熱塑性塑膠可接著較佳為PP、聚乙烯(PE)、聚碳酸酯(PC)、聚氯乙烯(PVC)、環氧樹脂、異氰酸酯樹脂、丙烯酸酯樹脂、聚酯樹脂或聚醯胺。
當所用之外部材料係熱固性塑膠或彈性體,前述纖維係藉由滲入反應性樹脂而加工,例如聚胺基甲酸酯樹脂、環氧樹脂、酚樹脂、乙烯基樹脂或(甲基)丙烯酸酯樹脂,
且隨後硬化以得到複合材料。
該泡沫芯體之材料係由P(M)I提供,較佳為PMI。這些P(M)I泡沫體也稱為剛性泡沫體,且特徵為特有之穩健性。該P(M)I泡沫體正常依兩段式方法製造:a)鑄造聚合物之製造,及b)前述鑄造聚合物之形成。
該鑄造聚合物之製造開始時製造單體混合物,該單體混合物包含主要組分,(甲基)丙烯酸及(甲基)丙烯腈,較佳為依2:3至3:2之莫耳比。其他共單體也可使用,例子係丙烯酸或甲基丙烯酸之酯類、苯乙烯、順丁烯二酸或衣康酸和其酸酐或乙烯基吡咯烷酮。然而,在此該共單體之比例不高於30重量%。也可使用小量之交聯單體,例如丙烯酸烯丙酯。然而,該量較佳應為至多0.05至2.0重量%。
該共聚合混合物也包含發泡劑,該發泡劑於約150至250℃之溫度,分解或汽化且因此形成氣相。該聚合反應發生於低於此溫度,且該鑄造聚合物因此包含潛在發泡劑(latent blowing agent)。該聚合反應有益地發生於二玻璃板之間的塊模(block mould)。為了製造發泡板,根據先前技藝這於是緊接著於第二步驟時於適當溫度形成該鑄造聚合物。這些PMI泡沫體之製法原則上係熟悉此技藝者已知者且能舉例來說於EP 1 444 293、EP 1 678 244或WO 2011/138060中見到。可能特別值得一提之PMI泡沫體係Evonik Industries AG之ROHACELL®等級。有關製造及加工丙烯醯亞胺泡沫體被視為與該PMI泡沫體類似。然
而,丙烯醯亞胺泡沫體因為毒物學顯然比其他泡沫體材料更不宜。
該剛性泡沫體材料之密度能相對任意選用。能使用之P(M)I泡沫體內的密度範圍實例係20至250kg/m3,較佳為25至220kg/m3。特佳為使用密度為30至200kg/m3之PMI泡沫體。
本發明之輕質結構材料的蜂巢較佳能由紙、塑膠或金屬構成。在此能使用之特定金屬係鋁、鎂、鈦和鋼。其他特別適合之實施態樣舉例來說係使用滲入酚樹脂且接著硬化之聚芳醯胺紙。同樣特佳為該蜂巢係由鋁構成。
該個別蜂巢之形狀、直徑和高度原則上係熟悉該輕質結構領域者已知者,且能輕易應用於本發明。唯一重要之因子係該蜂巢能某程度藉由後續泡沫體材料之未發泡或預發泡粒子填充。
較佳為當垂直觀看該蜂巢時其係方形,不規則四邊形、六角形或八角形。也可想到不同形狀之組合。較佳為藉由大約同尺寸之蜂巢覆蓋該區域的設計。此類型之蜂巢的蜂巢最厚點處之側面間距離較佳為0.1至20cm,特別是1至10cm。相對之下,該蜂巢之高度能絕對任意地選用。必定得考慮之唯一因子係在該發泡程序之前,個別蜂巢之體積及該泡沫體之期望密度自然限定填入個別蜂巢之能發泡粒子的量。此量能輕易地由熟悉此技藝者從蜂巢體積、所形成之材料本質、期望密度前述材料中之發泡劑濃度及發泡程序期間之溫度決定,且的確若所形成之材料的
組成已知則能確定該量而不需任何預備實驗。
所用之蜂巢材料的密度,還有該蜂巢之尺寸和壁厚度扮演決定本發明之輕質結構材料的重量還有機械性質之角色。該輕質結構材料能藉由選擇適當之P(M)I泡沫體和其性質(特別是密度)而相對於總重量減量或機械穩健性改良程度輕易地最佳化。
本發明不僅提供包含剛性P(M)I泡沫體之已述蜂巢,特別是還有包含泡沫體之蜂巢的製法。本發明之方法不僅限於包含P(M)I之蜂巢,還能用於其他未發泡狀態時呈微粒形式之能發泡塑膠。
用於製造包括含泡沫體之蜂巢的輕質結構材料之方法的特徵特別是具有下述步驟:a.將能發泡之粒子填入蜂巢材料,b.使該粒子發泡,其中該能發泡之粒子係由PE、PP、PMMA、PS或P(M)I構成。
先前所提供關於該包含剛性P(M)I泡沫體之蜂巢的描述在此同樣適於該蜂巢材料。
以上引用較佳特性提供之特性描述同樣適於該P(M)I或由彼製造之泡沫體。
PE泡沫體和PP泡沫體尤其為人所熟知的是於運輸容器中及當夾層材料之絕緣材料。PE泡沫體和PP泡沫體能包含填料,且大都能依20至200kg/m3之密度範圍自市場上購得。
相對之下,PMMA泡沫體之特徵為特別好之耐候性及
高耐UV性。然而,製造業至今仍未將PMMA泡沫體視為具有任何重大之重要性。
相對之下,聚苯乙烯(PS)係為眾所周知之泡沫體材料。當使用PS時,上述關於包含P(M)I之蜂巢結構的大部分優點沒有了,因為PS泡沫體具有更小許多之機械強度。然而,卻仍保有優於沒填充之蜂巢的主要優點:其進一步加工由於填充而顯著更容易。當液態樣脂能用以形成外層時這特別適用。
在本發明之方法中較佳為使用由P(M)I製造,特佳為由PMI製造,之能發泡的粒子。
P(M)I粒子較佳能藉由兩個替代例獲得。在第一替代例中,該P(M)I係如前述依P(M)I半成品之形式,特別是依板之形式,製造。藉由研磨能接著自此獲得依能輕易調整之粒徑的細粒。
在第二同樣較佳之替代例中該P(M)I粒子係懸浮聚合物。這些P(M)I懸浮聚合物之製法舉例來說能於2013年2月15日申請之申請案參考編號13155413.1的歐洲專利案中見到。
特佳為預發泡之粒子,特別是密度為25至220kg/m3,係填入該蜂巢。驚人的是,在此已發現當使用預發泡之粒子時後續以泡沫體填充該個別蜂巢特別均勻且因此具有特別好之機械性質。
該任意預發泡程序和步驟b.之發泡程序二者能藉熱及/或藉由微波達成。能用於此之分別加工參數取決於所用
之風泡劑、泡沫體材料、望期密度及蜂巢尺寸。這些參數能由熟悉此技藝者自已知之先前技藝輕易地推衍出來。
在該發泡程序時,當包含該粒子之蜂巢水平及/或垂直旋轉及/或移動時將獲得特別均勻之細孔分佈且因此於蜂巢內之均勻密度。特佳為水平旋轉,其能任意與其他移動結合。提供移動之適當設備能被輕易地設立於烘箱中。或者,前述設備舉例來說能具有被引至該蜂巢之微波來源。
較佳為本發明所製造之輕質結構材料的密度,特別是該包含P(M)I泡沫體之本發明的蜂巢,係30至350kg/m3,較佳為40至300kg/m3且特佳為50至250kg/m3。此密度不僅包含該蜂巢材料之壁,還有該泡沫體填充和任何未被佔據之空間。在附加外層之事件中,此密度適用於該芯材而非前述外層。
或者或此外,然而特佳地,步驟b.係於壓機中進行。此壓機之結構使得該泡沫體自該壓機移走之後與該蜂巢邊緣齊平。這意指理想上該壓機與該蜂巢之開式邊緣接觸。在此不需施加高壓。而是,足夠之壓力係能耐發泡程序之壓力者。
在另一步驟中,等到步驟b.完成之後,且跟在該步驟後面冷卻之後,該包含泡沫體之蜂巢能依據以上包含P(M)I泡沫體之蜂巢的描述藉由拼接、將插銷***穿過該材料或黏著接合,接合於一或二外層。
此刻,較佳為該外部材料附隨置於該壓機中之可供選
擇的實施態樣。利用此類型之程序,能任意省略任何其他黏著接合、拼接或將插銷***穿過該材料。也能提供黏著劑層給該外部材料。
該樹脂非常快速之硬化在此能藉由該壓機之模具殼體與該外部材料之間的直接接觸達成。用於使該樹脂固化之溫度取決於所用之特定樹脂且能由熟悉此技藝者輕易決定。這些溫度一般係為100至300℃。特別是,用於使該泡沫芯體發泡之較佳溫度,170至250℃,因此也適於大部分樹脂系統。在需要較高溫度之較不宜的事件中,該樹脂之固化能於另一個加熱單元中達成。
為了改善泡沫體芯材與外層之間的黏著力,能另外使用黏著促進劑。前述黏著促進劑可能存於該外層之基質材料中。或者,也可能在材料合併之前將該黏著促進劑施於該外層或該泡沫芯體之表面上。或者也能於此程序中使用適合之黏著劑。已經證明適合之特定黏著促進劑係聚酯類、聚醯胺類及聚(甲基)丙烯酸酯類。然而,也能使用熟悉此技藝者從複合材料製法得到之低分子量化合物,特別是按照用於外層之基質材料的需要。
能選用於本發明整個程序之加工參數取決於個別案例和其意圖中使用之系統設計,且也取決於所用之材料。其能由熟悉此技藝者利用少許預備實驗決定。
原則上,本發明之輕質結構材料或依據本發明之方法製造的輕質結構材料用途非常多。本發明所製造之輕質結構材料特別是能依量產,例如用於車身結構或汽車產業之
內部覆層、軌道車結構或造船之內部裝備零件、太空船、機械工程、製造運動裝備、家具結構或風輪機(wind turbine)之設計。
預發泡之PMI細粒係用於該蜂巢發泡程序。這是由粒徑<0.1mm之PMI細粒製造,該細粒係於烘箱中於200℃預發泡經過15分鐘且接著平均粒徑為約1mm。所用之PMI微粒係按照Evonik Industries之商品名ROHACELL RIMA的PMI泡沫體販售之材料。所用之蜂巢係單元尺寸5mm且厚度13mm之聚芳醯胺蜂巢。該蜂巢之密度係50kg/m3。該蜂巢係切成某個尺寸使其能精確地套入具有金屬基板之金屬框架(尺寸16×16cm)。此金屬框架之高度相當於該蜂巢之厚度,且該蜂巢之上側因此與該框架齊平。將31g之先前預發泡之細粒均勻地填入前述蜂巢使該蜂巢之所有穴室包含達於約其高度一半的預發泡之微粒。利用此填充之蜂巢被PTFE膜覆蓋且係置於230℃之熱壓機中。將該壓機閉合(鎖模力50bar)。經過60分鐘之後,將該壓機冷卻至室溫且將該金屬框架和該PTFE膜移除。製得之產物係具有均勻PMI泡沫體填充之蜂巢結構。
類似於實施例1,但是將材料填入該蜂巢之方法使該
金屬框架之基板係先均勻地覆蓋著31g之預發泡的細粒,且接著將該蜂巢強迫推進此微粒均勻層直到其達到該金屬框架之基板。這使該蜂巢之穴室得到非常均勻之預發泡的微粒填充。該蜂巢發泡程序按照實施例1之方式進行。
Claims (18)
- 一種輕質結構材料,其特徵為該輕質結構材料具有包含聚(甲基)丙烯酸醯亞胺泡沫體(P(M)I)之蜂巢結構。
- 如申請專利範圍第1項之輕質結構材料,其中該包含P(M)I泡沫體之蜂巢採芯材板形式且於至少一側具有外層。
- 如申請專利範圍第2項之輕質結構材料,其中該外層係金屬板或木板或複合板,藉由拼接(stitching)或黏著接合或藉由針腳接合於該芯材。
- 如申請專利範圍第3項之輕質結構材料,其中該複合材料係由玻璃纖維、碳纖維、聚芳醯胺纖維(aramid fibre)或紡織纖維及聚胺基甲酸酯樹脂、聚酯樹脂、環氧樹脂、酚樹脂或(甲基)丙烯酸酯樹脂構成之材料。
- 如申請專利範圍第1至4項中任一項之輕質結構材料,其中該P(M)I泡沫體係密度為20至250kg/m3之PMI泡沫體。
- 如申請專利範圍第1至4項中任一項之輕質結構材料,其中該蜂巢係由紙、塑膠或金屬構成,且該包含P(M)I泡沫體之蜂巢的密度係30至350kg/m3。
- 如申請專利範圍第6項之輕質結構材料,其中該蜂巢係由鋁、鎂、鈦或鋼構成。
- 一種用於製造輕質結構材料之方法,其特徵為該方法具有下列步驟:a.將能發泡之粒子填入蜂巢結構, b.使該粒子發泡,其中該能發泡之粒子係由PE、PP、PMMA、PS或P(M)I構成。
- 如申請專利範圍第8項之方法,其中該能發泡之粒子係由P(M)I構成,較佳由PMI構成。
- 如申請專利範圍第9項之方法,其中該P(M)I粒子已經藉由研磨由P(M)I半成品預先製成粒狀。
- 如申請專利範圍第9項之方法,其中該P(M)I粒子係懸浮聚合物。
- 如申請專利範圍第8至11項中任一項之方法,其中於步驟a填入蜂巢之粒子係密度為25至250kg/m3之預發泡粒子。
- 如申請專利範圍第8至11項中任一項之方法,其中步驟b之發泡經熱反應及/或藉由微波進行。
- 如申請專利範圍第8至11項中任一項之方法,其中在該發泡期間以水平及/或垂直方式旋轉及/或移動包含該粒子之蜂巢。
- 如申請專利範圍第8至11項中任一項之方法,其中步驟b係由壓製機進行,且自該壓製機移出後,該泡沫體與該蜂巢之邊緣齊平。
- 如申請專利範圍第15項之方法,其中在該壓製機中該包含能發泡之粒子的蜂巢係由至少一外層覆蓋。
- 如申請專利範圍第16項之方法,其中該外層係呈預浸體嵌入且在步驟b中經由發泡使該外層同時硬化。
- 如申請專利範圍第15項之方法,其中該包含泡 沫體之蜂巢係藉由拼接、針腳或黏著接合接合於如申請專利範圍第3或4項所述之至少一外層。
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JP7428716B2 (ja) | 2019-01-16 | 2024-02-06 | エボニック オペレーションズ ゲーエムベーハー | 発泡材料を製造するための新規の発泡法 |
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WO2017167197A1 (en) * | 2016-03-30 | 2017-10-05 | Evonik Specialty Chemicals (Shanghai) Co., Ltd. | Polymer compounds comprising poly (meth) acrylimide foam particles |
CN108884256A (zh) * | 2016-03-30 | 2018-11-23 | 赢创特种化学(上海)有限公司 | 包含聚(甲基)丙烯酰亚胺泡沫粒子的聚合物配混物 |
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