CN109562001A - 弹性附接热熔融粘合剂组合物及由其制备的一次性吸收制品 - Google Patents

弹性附接热熔融粘合剂组合物及由其制备的一次性吸收制品 Download PDF

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Publication number
CN109562001A
CN109562001A CN201780047700.8A CN201780047700A CN109562001A CN 109562001 A CN109562001 A CN 109562001A CN 201780047700 A CN201780047700 A CN 201780047700A CN 109562001 A CN109562001 A CN 109562001A
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China
Prior art keywords
weight
adhesive composition
propylene
hot
melt adhesive
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CN201780047700.8A
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English (en)
Inventor
C·布里赛诺
S·R·沃恩
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HB Fuller Co
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HB Fuller Co
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Abstract

本发明的特征在于基于烯烃聚合物的热熔融粘合剂组合物，所述热熔融粘合剂组合物可用于在一次性制品的制造中进行弹性附接。所述热熔融粘合剂包含约3重量％至约10重量％的由ASTM D1238(190℃，2.16kg)测得的熔融指数不大于约5的第一基于丙烯的共聚物、在190℃下粘度不大于约5000cps的第二基于丙烯的聚合物、软化点为至少约90℃的第一增粘剂、以及约5重量％至约20重量％的增塑剂。

Description

弹性附接热熔融粘合剂组合物及由其制备的一次性吸收制品
背景技术
在工业粘合剂领域，热熔融粘合剂通常用于将包括含有非织造基底的一次性吸收制品的多种制品粘结在一起，例如成人失禁产品、一次性尿布、卫生巾、床垫、宠物垫、医用敷料等。
在一次性吸收制品的制造中可以使用多种热熔融粘合剂。例如，在一次性尿布的制造中，粘合剂用于构造(例如，将底片粘结到非织造材料和任选的吸收垫)、弹性附接(例如，将弹性材料粘结到例如腿部或腰部区域中的底片上)以及芯稳定(例如，将粘合剂施加到吸收芯以增加芯的强度)中。
用聚烯烃聚合物配制的用于弹性附接应用的热熔融粘合剂尤其是在体温和应力下趋于具有比用苯乙烯嵌段共聚物(SBC)配制的那些高的蠕变。期望在用于弹性附接应用的热熔融粘合剂中使用聚烯烃聚合物，因为它们趋于具有较低的气味。
本行业中需要基于烯烃的热熔融粘合剂，其可用于弹性附接并且在应力下暴露于体温时提供可接受的蠕变。
发明内容
在一个方面，本发明的特征在于热熔融粘合剂组合物，该热熔融粘合剂组合物包含约3重量％至约10重量％的由ASTM D1238(190℃，2.16kg)测得的熔融指数不大于约5的第一基于丙烯的共聚物、在190℃下粘度不大于约5000cps的第二基于丙烯的聚合物、软化点为至少约90℃的第一增粘剂、以及约5重量％至约20重量％的增塑剂。
在一个实施方案中，第一增粘剂以约20重量％至约70重量％存在。在另一个实施方案中，第一增粘剂具有至少约110℃的软化点。在又一个实施方案中，第一基于丙烯的共聚物具有不小于约10的乙烯含量。在不同的实施方案中，第一基于丙烯的共聚物以约3重量％至约7重量％存在。
在一个实施方案中，第二基于丙烯的聚合物在190℃下具有不大于约3,000cps或甚至不大于约2,000cps的粘度。在另一个实施方案中，第二基于丙烯的聚合物以约7重量％至约20重量％存在。在又一个实施方案中，热熔融粘合剂组合物还包含第三聚合物。
在一个实施方案中，第一基于丙烯的共聚物、第二基于丙烯的聚合物、第三聚合物、第一增粘剂和增塑剂构成粘合剂组合物的至少90％。在另一个实施方案中，第一基于丙烯的共聚物和第二基于丙烯的聚合物的总含量不小于约10重量％。
在一个实施方案中，热熔融粘合剂组合物在177℃下具有约3,000cps至约20,000cps的粘度。在不同的实施方案中，热熔融粘合剂具有不大于35％的蠕变(37.8℃，4小时)。
在另一方面，本发明的特征在于一次性吸收制品，该一次性吸收制品包括：第一基底和弹性材料；以及粘合剂组合物，该粘合剂组合物包含约3重量％至约10重量％的由ASTMD1238(190℃，2.16kg)得出的熔融指数不大于约5的第一基于丙烯的共聚物、在190℃下粘度不大于约5000cps的第二基于丙烯的聚合物、熔点为至少90℃的增粘剂、以及约5重量％至约20重量％的增塑剂，其中粘合剂组合物与弹性材料和第一基底接触。
在一个实施方案中，一次性吸收制品选自包括以下项的组：成人失禁产品和尿布。在不同的实施方案中，一次性吸收制品是尿布。在另一个实施方案中，一次性吸收制品是成人失禁产品。在又一个实施方案中，粘合剂组合物将弹性材料粘结到第一基底，从而产生抗蠕变皱褶。
快凝结速率、高拉伸强度和低蠕变使得使用本发明热熔融粘合剂组合物在一次性吸收制品的制造中进行弹性附接成为可能。
热熔融粘合剂组合物
本发明的特征在于基于烯烃聚合物的热熔融粘合剂组合物，该热熔融粘合剂组合物可用于在一次性制品的制造中进行弹性附接。热熔融粘合剂包含约3重量％至约10重量％的由ASTM D1238(190℃，2.16kg)测得的熔融指数不大于约5的第一基于丙烯的聚合物、在190℃下粘度不大于约5000cps的第二基于丙烯的聚合物、软化点为至少约90℃的第一增粘剂、以及约5重量％至约20重量％的增塑剂。
第一基于丙烯的聚合物、第二基于丙烯的聚合物、第三聚合物、第一增粘剂和增塑剂可构成组合物的至少80重量％、至少85重量％、至少90重量％、或甚至至少95重量％。
第一基于丙烯的聚合物、第二基于丙烯的聚合物、第三聚合物、第一增粘剂、第二增粘剂和增塑剂可构成组合物的至少80重量％、至少85重量％、至少90重量％、或甚至至少95重量％。
当在177℃的温度下测量时，热熔融粘合剂组合物的粘度为约3,000cps至约30,000cps、约3,000cps至约20,000cps、或甚至约5,000cps至约15,000cps。
热熔融粘合剂组合物可具有不大于约35％、不大于约30％或甚至不大于约25％的蠕变(37.8℃，4小时)。
聚合物
粘合剂组合物包含至少两种不同的基于丙烯的聚合物。基于丙烯的聚合物被定义为包含至少50重量％的丙烯的聚合物。可用于第一聚合物和/或第二聚合物的基于丙烯的聚合物包括丙烯均聚物。另选地，两种不同的基于丙烯的聚合物中的一者或两者可为丙烯与一种或多种其它单体(例如乙烯、丁烯、戊烯、辛烯等)的共聚物。基于丙烯的聚合物可完全基于烯烃，即不包含任何官能团。基于丙烯的聚合物可包含大于75重量％的丙烯，或甚至大于80重量％的丙烯。基于丙烯的聚合物可具有小于约5、小于约3、约1至约4、或甚至约2的多分散性(Mw/Mn)。可用的基于丙烯的聚合物可具有不大于约0.90、不大于约0.89、不大于约0.88、或甚至约0.86至约0.88的密度。可用的基于丙烯的聚合物包括单点(例如，茂金属)催化的基于丙烯的聚合物。
第一聚合物是基于丙烯的聚合物。第一聚合物可为基于丙烯的共聚物。第一基于丙烯的聚合物具有如由ASTM D1238(190℃，2.16kg)测得的不大于7、不大于5、约1至约7、或甚至约2至约5的熔融指数。
第一基于丙烯的聚合物具有大于约250000克/摩尔、大于约275000克/摩尔、或甚至约250000至约350000克/摩尔的Mw(使用可见于“实施例”部分中的高温GPC分子量分布分析测试方法得出)。
第一基于丙烯的聚合物可具有不小于约10重量％、不小于约12重量％、或甚至约10重量％至约20重量％的共聚单体含量。在一个实施方案中，共聚单体是乙烯。
第一基于丙烯的聚合物可以不大于约10重量％、不大于约8重量％、约3重量％至约10重量％、或甚至约3重量％至约7重量％存在于组合物中。可用的可商购获得的第一基于丙烯的聚合物包括得自德克萨斯州休斯敦的埃克森美孚化工公司(ExxonMobilChemical(Houston,Texas))的VISTAMAXX 6102。
第二聚合物是基于丙烯的聚合物。第二基于丙烯的聚合物在190℃下具有不大于约5000cps、不大于约3000cps、不大于约2000cps、或甚至约750cps至约3000cps的粘度。第二基于丙烯的聚合物可具有小于约60000克/摩尔、小于约50000克/摩尔、或甚至约20,000克/摩尔至约60,000克/摩尔的Mw(使用可见于“实施例”部分中的高温GPC分子量分布分析测试方法得出)。
第二基于丙烯的聚合物可具有不大于约12重量％、不大于约10重量％、约5重量％至约15重量％、或甚至约0重量％至约12重量％的共聚单体含量。
第二基于丙烯的聚合物可以不小于约7重量％、不小于约10重量％、约7重量％至约20重量％、或甚至约10重量％至约18重量％存在于粘合剂组合物中。可用的可商购获得的第二基于丙烯的聚合物包括得自瑞士穆滕茨的科莱恩国际公司(ClariantInternational Ltd.(Muttenz,Switzerland))的LICOCENE PP6102和LICOCENE PP2602以及得自德克萨斯州休斯敦的埃克森美孚化工公司(ExxonMobil Chemical(Houston,Texas))的VISTAMAXX 8880。
第一基于丙烯的聚合物和第二基于丙烯的聚合物的总含量可为不小于约10重量％、约10重量％至约30重量％、或甚至约12重量％至约25重量％。
热熔融粘合剂还可包含第三聚合物。第三聚合物可为烯烃。第三聚合物可选自基于乙烯的聚合物和基于丙烯的聚合物。第三聚合物可具有如由ASTM D1238(190℃，2.16kg)测得的大于7、约8至约50、或甚至约8至20的熔融指数。第三聚合物可用于向粘合剂中建立强度，同时对粘度的影响不如第一聚合物那样多。当存在第三聚合物时，其可以约5重量％至约25重量％、约7重量％至约20重量％、或甚至约7重量％至约15重量％存在。
可用的可商购获得的第一基于丙烯的聚合物包括得自德克萨斯州休斯敦的埃克森美孚化工公司(ExxonMobil Chemical(Houston,Texas))的VISTAMAXX 6202。
增粘剂
热熔融粘合剂包含第一增粘剂和任选的第二增粘剂。
第一增粘剂和第二增粘剂可为至少部分氢化的。第一增粘剂和第二增粘剂的合适类别包括例如芳族、脂族和环脂族烃树脂、混合的芳族和脂族改性的烃树脂、芳族改性的脂族烃树脂以及它们的氢化的型式；萜烯、改性的萜烯、以及它们的氢化的型式；天然松香、改性的松香、松香酯、以及它们的氢化的型式；低分子量聚乳酸；以及它们的组合。可用的天然和改性的松香的示例包括脂松香、木松香、妥尔油松香、蒸馏松香、氢化的松香、二聚松香和聚合松香。可用的松香酯的示例包括例如浅色木松香的甘油酯、氢化的松香的甘油酯、聚合松香的甘油酯、天然和改性的松香的季戊四醇酯，该天然和改性的松香的季戊四醇酯包括浅色木松香的季戊四醇酯、氢化的松香的季戊四醇酯、妥尔油松香的季戊四醇酯和松香的酚改性的季戊四醇酯。
第一增粘剂在室温下为固体。第一增粘剂具有至少约90℃、至少约100℃、至少约110℃、至少约115℃、至少约125℃、或甚至约110℃至约150℃的软化点。可用的第一增粘剂可以多种商品名商购获得，包括例如得自德克萨斯州休斯敦的埃克森美孚化工公司(ExxonMobil Chemical Company(Houston,Texas))的ESCOREZ商品名系列(包括ESCOREZ 5600和5415)，以及得自田纳西州金斯波特的伊士曼化工公司(Eastman Chemical(Kingsport,Tennessee))的EASTOTAC商品名系列(包括EASTOTAC H-130)，以及得自俄亥俄州阿克伦的阿克洛化学公司(Akrochem Corporation(Akron,Ohio))的RESINALL R1030。
粘合剂组合物可包含约20重量％至约70重量％、约30重量％至约67重量％、或甚至约45重量％至约65重量％的第一增粘剂。
第二增粘剂的软化点可小于第一增粘剂的软化点。
增塑剂
热熔融粘合剂组合物包含增塑剂。合适的增塑剂包括例如环烷油、石蜡油(例如，环烷烃油)、矿物油、邻苯二甲酸酯、己二酸酯、烯烃低聚物(例如，聚丙烯、聚丁烯和氢化的聚异戊二烯的低聚物)、聚丁烯、聚异戊二烯、氢化的聚异戊二烯、聚丁二烯、苯甲酸酯、动物油、植物油(例如，蓖麻油、大豆油)、油的衍生物、脂肪酸的甘油酯、聚酯、聚醚、乳酸衍生物、固体增塑剂(例如，苯甲酸酯)以及它们的组合。在一个实施方案中，增塑剂是油。
可用的可商购获得的增塑剂包括得自印第安纳州印第安纳波利斯的卡路梅特殊产品合伙人公司(Calumet Specialty Products Partners,LP(Indianapolis,Indiana))的CALSOL 5550油、得自纽约州柏油村的索诺邦公司(Sonneborn(Tarrytown New York))的KAYDOL OIL、得自德克萨斯州休斯顿的埃克森美孚化工公司(Exxon Mobil ChemicalCompany(Houston,Texas))的PARAPOL聚丁烯、得自德国路德维希港的巴斯夫公司(BASF(Ludwigshafen,Germany))的OPPANOL聚异丁烯、得自英国萨里郡的Petrochem Carless公司(Petrochem Carless Limited(Surrey,England))的KRYSTOL 550矿物油、得自安大略省米西索加的加拿大石油润滑剂公司(Petro Canada Lubricants Inc.(Mississauga,Ontario))的PURETOL 15矿物油、以及得自田纳西州金斯波特的伊士曼化工公司(EastmanChemical Company(Kingsport,Tennessee))的BENZOFLEX 352(一种在室温下呈固体的苯甲酸酯增塑剂)。
增塑剂以不大于20重量％、不大于18重量％、约5重量％至约20重量％、或甚至约10重量％至约18重量％存在。
附加组分
粘合剂组合物任选地包含附加组分，包括例如稳定剂、抗氧化剂、附加聚合物(例如，苯乙烯嵌段共聚物、无定形聚α烯烃、聚乙烯共聚物)、附加增粘剂、蜡、粘附促进剂、紫外光稳定剂、着色剂(例如，颜料和染料)、填料、表面活性剂、共挤出涂层、包装膜、润湿指示剂、超吸收剂以及它们的组合。
可用的抗氧化剂包括例如季戊四醇四[3,(3,5-二叔丁基-4-羟基苯基)丙酸酯]、2,2'-亚甲基双(4-甲基-6-叔丁基苯酚)、亚磷酸盐(包括例如三-(对-壬基苯基)-亚磷酸盐(TNPP)和双(2,4-二-叔丁基苯基)4,4'-二亚苯基-二膦酸盐)、二-硬脂基-3,3'-硫代二丙酸酯(DSTDP)以及它们的组合。可用的抗氧化剂可以多种商品名商购获得，包括例如IRGANOX系列商品名，包括例如IRGANOX 1010、IRGANOX 565和IRGANOX 1076受阻酚抗氧化剂和IRGAFOS 168亚磷酸盐抗氧化剂(这些抗氧化剂均可购自新泽西州弗洛勒姆帕克的巴斯夫公司(BASF Corporation,Florham Park,New Jersey))，以及ETHYL 702 4,4'-亚甲基双(2,6-二叔丁基苯酚)。当存在时，粘合剂组合物优选包含约0.1重量％至约2重量％的抗氧化剂。
一次性吸收制品
可将粘合剂组合物施加于(即，使得其直接接触)或结合到多种基底中，包括例如膜(例如，聚烯烃(例如聚乙烯和聚丙烯)膜)、防粘衬垫、多孔基底、纤维素基底、片材(例如，纸材和纤维片)、纸材产品、织造和非织造纤维网、纤维(例如，合成聚合物纤维和纤维素纤维)和带材背衬。
粘合剂组合物还可用于多种应用和构造，包括例如一次性吸收制品，包括例如一次性尿布、成人失禁产品、卫生巾、医疗敷料(例如，伤口护理产品)、绷带、手术垫、宠物训练垫(例如，宠物垫)和肉类包装产品以及吸收制品的组件，包括例如吸收元件、吸收芯、不可渗透的层(例如，底片)、薄纸(例如，包装薄纸)、采集层以及织造和非织造纤维层(例如，顶片、吸收薄纸)及弹性件。
粘合剂组合物可用于由多种纤维制成的基底上，所述纤维包括例如天然纤维素纤维，诸如木浆、棉、丝绸和羊毛；合成纤维，诸如尼龙、人造丝、聚酯、丙烯酸类、聚丙烯、聚乙烯、聚氯乙烯、聚氨酯和玻璃；回收的纤维、以及它们的各种组合。
可使用多种应用技术将组合物施加于基底，所述技术包括例如狭缝涂布、喷涂(包括例如旋喷和随机喷涂)、丝网印刷、发泡、刻花辊、挤出和熔喷应用技术。
制备一次性吸收制品的方法
热熔融粘合剂组合物用于弹性附接应用，所述弹性附接应用包括将弹性材料(例如，股线、膜等)粘结到一次性吸收制品的部件。弹性材料可在处于拉伸形式时用热熔融粘合剂组合物进行涂布，然后粘结到膜(例如，聚乙烯、聚丙烯等)或非织造基底。涂布有热熔融粘合剂的弹性材料也可粘结在两个此类基底之间。一旦移除张力，该过程就产生抗蠕变皱褶。
粘合剂可另选地施加到膜或非织造基底，然后弹性材料粘结到其上。
热熔融粘合剂可在形成一次性吸收制品的耳部/突片中用作弹性附接粘合剂。
另选地，热熔融粘合剂还可用作弹性附接粘合剂以有助于使一次性吸收制品的腿部开口或腰部具有弹性。
本发明现在将通过以下实施例加以描述。除非另外指明，否则实施例中所述的所有份数、比率、百分比和量均按重量计。
实施例
测试工序
除非另外指明，否则用于实施例和整篇说明书的测试工序包括以下工序。表2和表3中所列的原材料的量以重量百分比计。
高温GPC分子量分布分析
使用高温HPLC系统及BHT稳定的1,2,4-三氯苯(TCB)流动相来获得表1中的每种聚合物的GPC分子量分布曲线。相对于聚苯乙烯标准品来计算分子量数据。
GPC系统：Agilent PL-GPC 220
流动相：用0.0125％BHT稳定的TCB
温度：160℃
柱：PLgel 10um mixed-B(3)
流速：1.0ml/min
进样体积：200μL
浓度：6.0mg/ml(0.009g/1.5mL)
粘度测试方法
根据标题为“Standard Test Method for Apparent viscosity of Adhesivesand Coating Materials(粘合剂和涂布材料的表观粘度的标准测试方法)”(1988年10月31日)的ASTM D-3236，使用博勒飞公司的RVDV 2型Thermosel粘度计(Brookfield Thermoselviscometer Model RVDV 2)和27号转子来测定粘度。结果以厘泊(cps)记录。
蠕变测定
粘结物制备
使用Nordson SURE WRAP喷嘴、177℃的施加温度和47.3毫克/股/米(1.2毫克/股/英寸)的涂层重量，将热熔融粘合剂以熔融形式施加到3根LYCRA 800分特股线(预拉伸到300％)。将粘合剂涂布在预拉伸的弹性股线上，然后将股线层合在非织造物(购自中西部过滤公司(Midwest Filtration LLC)的UNIPRO 45)与聚乙烯底片(购自克乐培公司(Clopay)的DH284)之间。
粘结测试
1.以非织造物面朝上的方式将多股线弹性附接层合物的一端钉到一片坚固的纸板的边缘上。
2.延伸样品达到100％完全伸展，注意不要过分延伸底片。
3.标出样品达到纸板上的300mm标记的位置。
4.松开样品直到样品标记达到纸板上的285mm标记，并且钉住该附接物的另一端。此时样品固定在完全伸展的95％。
5.在已以该相同方式附接至少五个样品之后，在附接物的每一端处切开弹性件的单独股线，从而允许股线能够在层合物内移动。注意不要切割整个聚乙烯片。
6.使锚定有试样的板在37.8℃(100℉)下适应四小时。
7.从烘箱移除板和试样，并且在弹性件仍粘结的地方标记聚乙烯(由附接物的皱褶部分表示)。
8.测量初始粘结的长度(285mm)以及四小时时弹性件仍粘结的地方的粘结长度；按照以下计算方式来计算蠕变百分比。
9.报告五个样品的平均值
计算
表1-聚合物特性
表2-实施例
比较例1* 对照例1 实施例1 实施例2 实施例3
VISTAMAXX 6102 2 3 5 5
VISTAMAXX 8880 14 13 16.9 12.5
VISTAMAXX 6202 14 13 9.1 12.5
EASTOTAC H130 60 59 54.5 55
CALSOL 550 10 12 14.5 15
177℃下的熔融粘度(cP) 10625 10200 8500 13100
蠕变-37.8℃(100℉)，4小时(％) 25 44 31 24 20
*比较例1是可从HB富勒公司(HB Fuller Company)商购获得的NW1002P ZP，其是一种基于苯乙烯嵌段共聚物(SBC)的粘合剂
表3-实施例
通过将各组分以表2中所示的百分比合并和混合于177℃下操作的曲拐式桨叶混合器中来制备粘合剂组合物。
添加剂行中的量包括存在于粘合剂中的抗氧化剂、共挤出涂层和包装膜的总量。
其它实施方案在权利要求书的范围内。

Claims (15)

1.一种热熔融粘合剂组合物，包含：
a.约3重量％至约10重量％的由ASTM D1238(190℃，2.16kg)测得的熔融指数不大于约5的第一基于丙烯的共聚物，
b.在190℃下粘度不大于约5000cps的第二基于丙烯的聚合物，
c.软化点为至少约90℃的第一增粘剂，以及
d.约5重量％至约20重量％的增塑剂。
2.根据权利要求1所述的热熔融粘合剂组合物，其中所述第一增粘剂以约20重量％至约70重量％存在。
3.根据权利要求1所述的热熔融粘合剂组合物，其中所述第一增粘剂具有至少约110℃的软化点。
4.根据权利要求1所述的热熔融粘合剂组合物，其中所述第一基于丙烯的共聚物具有不小于约10的乙烯含量。
5.根据权利要求1所述的热熔融粘合剂组合物，其中所述第一基于丙烯的共聚物以约3重量％至约7重量％存在。
6.根据权利要求1所述的热熔融粘合剂组合物，其中所述第二基于丙烯的聚合物在190℃下具有不大于约3,000cps的粘度。
7.根据权利要求1所述的热熔融粘合剂组合物，其中所述第二基于丙烯的聚合物以约7重量％至约20重量％存在。
8.根据权利要求1所述的热熔融粘合剂组合物，还包含第三聚合物。
9.根据权利要求9所述的热熔融粘合剂组合物，其中所述第一基于丙烯的共聚物、所述第二基于丙烯的聚合物、所述第三聚合物、所述第一增粘剂和所述增塑剂构成所述粘合剂组合物的至少90％。
10.根据权利要求1所述的热熔融粘合剂组合物，其中所述第一基于丙烯的共聚物和所述第二基于丙烯的聚合物的总含量不小于约10重量％。
11.根据权利要求1所述的热熔融粘合剂组合物，所述热熔融粘合剂组合物在177℃下具有约3,000cps至约20,000cps的粘度。
12.根据权利要求1所述的热熔融粘合剂组合物，所述热熔融粘合剂组合物具有不大于35％的蠕变(37.8℃，4小时)。
13.一种一次性吸收制品，包括：
a.第一基底，
b.弹性材料，以及
c.粘合剂组合物，所述粘合剂组合物包含：
i.约3重量％至约10重量％的由ASTM D1238(190℃，2.16kg)得出的熔融指数不大于约5的第一基于丙烯的共聚物，
ii.在190℃下粘度不大于约5000cps的第二基于丙烯的聚合物，
iii.熔点为至少90℃的增粘剂以及
iv.约5重量％至约20重量％的增塑剂；
其中所述粘合剂组合物与所述弹性材料和所述第一基底接触。
14.根据权利要求13所述的一次性吸收制品，其中所述一次性吸收制品选自成人失禁产品和尿布。
15.根据权利要求13所述的一次性吸收制品，其中所述粘合剂组合物将所述弹性材料粘结到所述第一基底，从而产生抗蠕变皱褶。
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