CN102378621A - 剥离性洁牙剂组合物及其使用方法 - Google Patents
剥离性洁牙剂组合物及其使用方法 Download PDFInfo
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- CN102378621A CN102378621A CN2009801585857A CN200980158585A CN102378621A CN 102378621 A CN102378621 A CN 102378621A CN 2009801585857 A CN2009801585857 A CN 2009801585857A CN 200980158585 A CN200980158585 A CN 200980158585A CN 102378621 A CN102378621 A CN 102378621A
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- dentifrice composition
- granule
- agent
- dentifrice
- oral
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Abstract
本申请描述含有多种颗粒和口腔可接受的媒介物的剥离性洁牙剂组合物。所述颗粒含有至少一种聚合物粘合剂。组合物包含至少一种平均粒径为0.01mm-4mm的研磨剂。还包括使用该组合物剥离口腔软组织的方法。
Description
发明背景
将机械剥离用于皮肤和表皮的益处为个人护理领域所熟知。然而，涉及口腔护理的专利和文献已经关注“脱落(sloughing)”的负面影响和剥落速度的急剧增加。已经提出常见洁牙表面活性剂使口腔和胃粘膜不适，甚至认为其促成牙周病，因为据说其造成慢性炎症和口腔粘膜脱落，从而促进致病微生物引起的感染。
化学剥离为皮肤健康领域所熟知，并常常涉及采用可加速脱皮(desquamination)速度的物质。已知pH为3-4的α或β羟基酸可增加个人护理产品中的酶过程的活性，但对口腔应用可能太过于侵蚀性。也已经报道了蛋白水解酶在减少口腔生物膜中的用途，但远未公开作为软组织剥离剂(exfoliant)的用途。
发明简述
本发明的实施方案包括将提供由剥离口腔粘膜引起的积极效果的洁牙剂组合物。
所描述的剥离性洁牙剂组合物含有多种颗粒和口腔可接受的媒介物。颗粒包含至少一种聚合物粘合剂，组合物包含至少一种平均粒径为0.01mm-4mm的研磨剂。还包括用组合物剥离口腔软组织的方法。
所描述的口腔软组织剥离系统包含如上所述的组合物和实现剥离活动的口腔护理工具。
发明详述
如全文所用的范围用作描述在该范围内的各个数值和每一个数值的简写。可选择在该范围内的任何值作为该范围的端点。
在某些实施方案中，本发明的剥离性洁牙剂组合物包含含有增稠剂和增塑性的颗粒。在某些实施方案中，本发明的洁牙剂组合物可应用于使用者的口腔，以剥离或增加口腔的脱屑(desquamation)。
术语“洁牙剂”应包括单独或组合的牙膏、牙胶(gels)和漂洗剂。洁牙剂组合物可为任何想要的形式，例如但不限于，带深条纹的(deepstriped)、带表面条纹的(surface striped)、多层的或牙胶和牙膏的任何组合。洁牙剂组合物的各组分的载体可包括如下所述的适用于口腔的任何口腔可接受的媒介物。洁牙剂颗粒和携带颗粒的媒介物在下文描述。
在某些实施方案中，洁牙剂组合物包括颗粒。
在某些实施方案中，颗粒可包括至少一种增稠剂。适用的增稠剂的实例包括，但不限于羟丙基甲基纤维素(HPMC)、羟丙基纤维素(HPC)、甲基纤维素和玉米淀粉中的一种或多种。在某些实施方案中，所述颗粒包括30-95％重量的量的增稠剂。在其它实施方案中，颗粒包含50-85％重量的量的增稠剂。在一个实施方案中，颗粒包含75％重量的量的增稠剂。
在某些实施方案中，颗粒包含至少一种增塑剂。适用的增塑剂的实例包括但不限于丙二醇、甘油和三醋精。在某些实施方案中，颗粒包含5-35％重量的量的增塑剂。在另一个实施方案中，颗粒包含10-20％重量的量的增塑剂。
在某些实施方案中，颗粒是研磨剂。在某些实施方案中，颗粒包括物理研磨剂。在某些实施方案中，物理研磨剂是二氧化硅。在某些实施方案中，颗粒包含5-50％重量的量的物理研磨剂。在某些实施方案中，颗粒包括15-30％重量的量的物理研磨剂。
在某些实施方案中，颗粒以组合物的1-5％重量的量存在。在某些实施方案中，研磨剂颗粒制剂以洁牙剂组合物的1％重量的量存在。
如本文所用，术语“口腔可接受的媒介物”将包括适用的媒介物，它可用来以安全和有效的方式将上述颗粒应用于口腔。这类媒介物可包括，但不限于，原料诸如氟化物离子源、另外的抗牙结石剂(anti-calculus agents)、缓冲剂、其它研磨材料、过氧化物源、碱金属碳酸氢盐、增稠材料、湿润剂、水、表面活性剂、矫味系统(flavorsystem)、增甜剂、着色剂，以及它们的混合物。在某些实施方案中，媒介物可包括牙膏、牙粉、预防糊剂(prophylaxis pastes)、牙胶、漂洗剂、锭剂、口胶剂(gums)等的常用组分。
在某些实施方案中，口腔可接受的媒介物包括水。
口腔可接受的媒介物还可包括湿润剂。在某些实施方案中，湿润剂包括甘油或山梨醇或烷撑二醇诸如聚乙二醇或丙二醇。在某些实施方案中，湿润剂以洁牙剂组合物的15-80％重量的量存在。在其它实施方案中，湿润剂以54-70％重量的量的存在。
口腔可接受的媒介物可包括无机或天然或合成增稠剂或胶凝剂。在某些实施方案中，增稠剂或胶凝剂以3.5-7％重量的量存在。在某些实施方案中，洁牙剂组合物中含有适当量的增稠剂以悬浮研磨颗粒或小珠。在某些实施方案中，洁牙剂组合物中含有适当量的增稠剂以形成可挤压、保持形状的产物，它能自管中挤到牙刷上且不会落在刷毛之间，而且相反将在其上基本保持其形状。洁牙剂组合物的适用的增稠剂或胶凝剂可包括无机增稠二氧化硅(可以商品名Zeodent 165得自Huber Corporation)、爱尔兰苔、角叉菜、黄蓍胶和聚乙烯吡咯烷酮。
在某些实施方案中，口腔可接受的媒介物包含至少一种表面活性剂。适用的表面活性剂可包括，但不限于，高级脂肪酸单硫酸甘油一酯(fatty acid monoglyceride monosulfates)的水溶性盐，诸如氢化椰子油脂肪酸的单硫酸化(monosulfated)甘油一酯的钠盐、椰油酰氨基丙基甜菜碱(cocamidopropyl betaine)、高级烷基硫酸盐诸如月桂基硫酸钠、烷基芳基磺酸盐诸如十二烷基苯磺酸钠、高级烷基磺基乙酸盐、月桂基磺基乙酸钠、1，2-二羟基丙烷磺酸盐的高级脂肪酸酯，和低级脂族氨基羧酸化合物的基本饱和的高级脂肪族酰基酰胺(acyl amides)，诸如脂肪酸、烷基或酰基等基团中具有12-16个碳的那些酰胺。适用的酰胺的实例可包括N-月桂酰基肌氨酸和N-月桂酰基肌氨酸、N-肉豆蔻酰基肌氨酸或N-棕榈酰基肌氨酸的钠、钾和乙醇胺盐。
在某些实施方案中，表面活性剂以0.1-5.0％重量的量存在于洁牙剂组合物中。在其它实施方案中，表面活性剂以0.45-2.5％重量的量存在于洁牙剂组合物中。在某些实施方案中，表面活性剂以0.45-2.5％重量的量存在于洁牙剂组合物中。
洁牙剂组合物还可含有粘合剂。适用的粘合剂的实例可包括，但不限于，海生胶体(marine colloids)，羧乙烯基聚合物，角叉菜胶，淀粉，水溶性纤维素醚诸如羟乙基纤维素、羧甲基纤维素(羧甲纤维素)、羟丙基甲基纤维素和它们的盐(例如，羧甲纤维素钠)，天然树胶诸如刺梧桐树胶、黄原胶、阿拉伯树胶和黄蓍胶，壳聚糖、胶态硅酸铝镁和胶态二氧化硅。在某些实施方案中，粘合剂以组合物的0.1-0.70％重量的量存在。
洁牙剂组合物也可包含矫味剂或矫味剂的混合物，包括天然或合成的矫味剂，诸如矫味油、矫味醛、酯、醇、类似原料，及其组合。适用的矫味剂的实例可包括香草醛、留兰香油、桂皮油、冬青油(水杨酸甲酯)、薄荷油、丁香油、茴香油、桉油、柑桔油、果油和精油。在某些实施方案中，洁牙剂组合物包含矫味剂诸如柠檬油精、薄荷酮、香芹酮、甲醇、茴香脑、桉油、桉油精、丁香酚、桂皮、oxanone、α-紫罗兰酮、丙烯基乙基愈创木酚(propenyl guaiethol)、百里酚、里哪醇、苯甲醛、肉桂醛、N-乙基-p-薄荷烷-3-甲酰胺、N-2，3-三甲基-2-异丙基丁酰胺、3，1-薄荷氧基丙烷(menthoxypropane)-1，2-二醇、肉桂醛甘油缩醛(CGA)、薄荷酮(methone)甘油缩醛(MGA)和桉树脑。
在某些实施方案中，洁牙剂组合物还可包含α和β羟基酸。羟基酸可加强存在于口腔中的天然生成的酶的作用。在某些实施方案中，洁牙剂组合物可包含羟基酸，诸如包含乳酸、乙醇酸和中和的水杨酸中的至少一种。在其它实施方案中，洁牙剂组合物可包含担负分解外细胞层的胰蛋白酶和蛋白酶。
在某些实施方案中，洁牙剂组合物包含0.05-5％重量的量的羟基酸。在其它实施方案中，洁牙剂组合物包含0.1-1％重量的量的羟基酸。
在某些实施方案中，洁牙剂组合物还可包含研磨剂。研磨剂可起到剥离的机械和物理工具的作用并增加口腔粘膜的脱落。在某些实施方案中，研磨剂分布遍及口腔可接受的媒介物中，或者它存在于颗粒中。
在某些实施方案中，洁牙剂组合物包含二氧化硅研磨剂。适用的研磨剂的实例包括，但不限于，二氧化硅研磨剂诸如沉淀二氧化硅、偏磷酸钠、偏磷酸钾、磷酸三钙、二水合磷酸二钙、硅酸铝、煅烧氧化铝、膨润土或其它硅质材料(siliceous materials)、微粒状热固性树脂诸如三聚氰胺、酚醛和脲醛，和交联聚环氧化物和聚酯。
研磨剂可以任何适当量存在。在某些实施方案中，这类研磨剂以1-40％重量的量存在。在其它实施方案中，这类研磨剂以18-20％重量的量存在。
在某些实施方案中，洁牙剂组合物包括研磨小珠。适用的可通过商业途径得到的研磨小珠的实例包括来自Presperse
的那些，诸如Microwhite
50。在某些实施方案中，研磨小珠的直径为0.1mm-5mm。在某些实施方案中，研磨小珠的直径为1mm-2mm。在某些实施方案中，研磨小珠以0.1-10％重量的量存在。在其它实施方案中，研磨小珠以0.2-3％重量的量存在。
为制备、稳定性、美感、疗效、消费者要求等理由，可在洁牙剂组合物中包含其它添加剂。示例性添加剂包括其它所有常规的洁牙剂添加剂、粘度调节剂、稀释剂、泡沫调节剂、唾液刺激剂、脱敏剂、增白剂、酶、pH调节剂、口感剂、甜味剂、着色剂、遮光剂和口气清新剂。其它示例性试剂可包括亚氯酸盐离子试剂、三氯生、5-氯-2-(2，4-二氯苯氧基)-酚、氯己定、阿来西定、海克替啶、血根碱、苯扎氯铵、水杨酰苯胺、度米芬、西吡氯铵、氯化十四烷基吡啶
氯化N-十四烷基-4-乙基吡啶
奥替尼啶、地莫匹醇、辛哌醇、哌啶子基衍生物、乳链菌肽、锌离子剂、亚锡离子剂、精油、呋喃酮、胞壁分解酶、溶菌酶、牙斑基质抑制剂、葡聚糖酶、牙斑葡聚糖酶、细菌素、人富组蛋白(histatins)、防卫素、杀菌肽、沃格孟汀(augmentin)、阿莫西林、四环素、多西环素、米诺环素、甲硝唑、新霉素、卡那霉素、克林霉素、氯化锶、硝酸钾、氟化物离子剂、薄荷油、叶绿素、利多卡因、苯佐卡因、氨基酸和过氧化物。
在某些实施方案中，洁牙剂组合物是糊剂或牙胶剂。可在洁牙剂组合物中包含适当量的增稠剂以悬浮颗粒或研磨小珠。在某些实施方案中，在洁牙剂组合物中含有适当量的增稠剂以形成可挤出、保持形状的产品，它可自管中挤出到牙刷上，且不会落在刷毛间，反而会在其上基本保持其形状。
如上所述的洁牙剂组合物可应用于口腔软组织。在某些实施方案中，应用洁牙剂组合物剥离口腔粘膜，包括内颊、舌头和齿龈细胞。在某些实施方案中，洁牙剂组合物通过机械/物理方式剥离。在某些实施方案中，洁牙剂组合物通过化学改变口腔的脱屑速度剥离。在某些实施方案中，应用洁牙剂组合物降低唾液中的总细菌负荷，局部细胞群体将会下降，无论是涂敷还是刷牙。
在某些实施方案中，将洁牙剂组合物应用于口腔提供至少一种以下结果：由于口腔厌氧菌蛋白水解的细菌代谢产生的临床减少挥发性硫化合物(VSC)所带来清新口气；由于全部口腔细菌和舌头/内颊细菌的减少带来的抗菌效果；因通过衰老技术使相对菌龄下降带来的“年轻口腔”；炎症减轻；口胶刺激导致血流向口胶增加，从而增加唾液流动；减少在舌头后部上菌斑的形成；提高粘膜的“呼吸”能力；改善其它成分的沉积；增加沉积活动的保留时间；和缓解早晨口臭/口气。因此，可用洁牙剂组合物保持口腔健康并治疗和预防口腔疾病。
在某些实施方案中，洁牙剂组合物可包含颗粒和α或β羟基酸。在某些实施方案中，颗粒和α或β羟基酸的组合协同剥离和增加口腔粘膜的脱落。
在某些实施方案中，洁牙剂组合物是牙膏和/或牙胶。
口腔软组织的剥离系统也包括在本发明的实施方案中。该系统可包含如上所述的任何变化形式的剥离性洁牙剂组合物，以及将洁牙剂应用于口腔软组织的口腔护理工具。例如，口腔护理工具可为舌头清洁器、牙刷、药签、海绵、指套、棉签(stick)、牙托和磨带(strip)。所述工具可由本领域已知的任何材料，诸如，塑料、树脂、木材、织物、聚合物、海绵、纸、箔、薄膜、金属和橡胶制得。包含于系统中的口腔护理工具可为本领域任何已知的或开发的。如果想要，人们可以希望包括这样的口腔护理工具，其包括剥离洁牙剂可能放于其中或其上的贮库、空腔或其它空间。
实验性实施例
实施例1：颗粒制剂
表1：剥离或增加脱落的颗粒制剂
| 成分 | 颗粒A，wt％ | 颗粒B，wt％ | 颗粒C，wt％ |
| 平均粒度 | 1mm | 0.75mm | 0.1mm |
| 羟丙基甲基纤维素 | 50 | 35 | 0 |
| 羟丙基纤维素(HPC) | 0 | 0 | 60 |
| 甲基纤维素 | 0 | 20 | 0 |
| 玉米淀粉 | 0 | 30 | 15 |
| 二氧化硅，AC43 | 30 | 0 | 15 |
| 增塑剂如丙二醇、甘油、三醋精等 | 20 | 15 | 10 |
| 合计 | 100 | 100 | 100 |
根据以上配方为制备以下实施例的颗粒剂。
实施例2：含有1％颗粒A的洁牙剂组合物
根据以下配方制备洁牙剂组合物：
表2：含有1％颗粒A的试样
| 成分 | ％重量 |
| 钠CMC | 0.65 |
| 聚乙二醇600(PEG-12) | 3.0 |
| 山梨醇 | 55.441 |
| 糖精钠 | 0.3 |
| 氟化钠 | 0.24 |
| 焦磷酸四钠 | 0.5 |
| FD&C蓝#1染料(1％在水中) | 0.4 |
| 二氧化硅研磨剂(Zeodent 115) | 20 |
| 二氧化硅增稠剂(Zeodent 165) | 4.25 |
| 矫味油 | 1.15 |
| 月桂基硫酸钠，100％ | 1.5 |
| 椰油酰氨基丙基甜菜碱 | 0.45 |
| 颗粒A | 1.0 |
| 水 | Q.S. |
实施例3：含有3％颗粒B的洁牙剂组合物
根据以下配方制备洁牙剂组合物：
表3：含有3％颗粒B的试样
| 成分 | ％重量 |
| CP纯净水 | 6 |
| 糖精钠 | 0.35 |
| 氟化钠 | 0.243 |
| 甘油 | 20 |
| 丙二醇 | 0.5 |
| 钠CMC | 1.1 |
| 角叉菜胶 | 0.5 |
| 绿染料溶液 | 0.2 |
| 山梨醇 | 20.35 |
| CP纯净水 | 5.485 |
| Gantrez S-97液体形式 | 15 |
| NaOH 50％ | 1.2 |
| 二氧化硅研磨剂 | 18.5 |
| 二氧化硅增稠剂 | 3 |
| 三氯生 | 0.3 |
| 香料 | 1.6 |
| SLS，29.0％ | 5.172 |
| 中和水杨酸 | 0.5 |
| 颗粒B | 3 |
| 合计 | 100％ |
实施例4：含有5％颗粒C的洁牙剂组合物
根据表4中的配方制备洁牙剂组合物。
表4：含有5％颗粒C的试样
| 成分 | ％重量 |
| 钠CMC | 0.65 |
| 聚乙二醇600(PEG-12) | 3.0 |
| 山梨醇 | 51.341 |
| 糖精钠 | 0.3 |
| 氟化钠 | 0.24 |
| 焦磷酸四钠 | 0.5 |
| FD&C蓝#1染料(1％在水中) | 0.4 |
| 二氧化硅研磨剂(Zeodent 115) | 20 |
| 二氧化硅增稠剂(Zeodent 165) | 4.25 |
| 矫味油 | 1.15 |
| 月桂基硫酸钠，100％ | 1.5 |
| 椰油酰氨基丙基甜菜碱 | 0.45 |
| 乳酸 | 0.1 |
| 颗粒C | 5.0 |
| 水 | Q.S. |
Claims (14)
1.一种剥离性洁牙剂组合物，其包含：
(A)多种颗粒，其中的颗粒包含至少一种聚合物粘合剂；和
(B)口腔可接受的媒介物，其中所述颗粒和口腔可接受的媒介物中的至少一种还包含至少一种具有0.01mm-4mm平均粒径的研磨剂。
2.权利要求1的洁牙剂组合物，其中的颗粒还包含选自羟丙基甲基纤维素、羟丙基纤维素(HPC)、甲基纤维素和玉米淀粉的增稠剂。
3.权利要求1的洁牙剂组合物，其中的颗粒还包含选自丙二醇、甘油和三醋精的增塑剂。
4.权利要求1的洁牙剂组合物，其中至少一种研磨剂包含二氧化硅。
5.权利要求1的洁牙剂组合物，其还包含羟基酸。
6.权利要求5的洁牙剂组合物，其中的羟基酸选自乳酸、乙醇酸和中和的水杨酸。
7.权利要求1的洁牙剂，其还包含蛋白水解酶。
8.权利要求1的洁牙剂，其还包含选自亚氯酸盐离子试剂、三氯生、5-氯-2-(2，4-二氯苯氧基)-酚、氯己定、阿来西定、海克替啶、血根碱、苯扎氯铵、水杨酰苯胺、度米芬、西吡氯铵、氯化十四烷基吡啶
氯化N-十四烷基-4-乙基吡啶
奥替尼啶、地莫匹醇、辛哌醇、哌啶子基衍生物、乳链菌肽、锌离子剂、亚锡离子剂、精油、呋喃酮、胞壁分解酶和溶菌酶的物质。
9.权利要求1的洁牙剂，其还包含选自牙斑基质抑制剂、葡聚糖酶、牙斑葡聚糖酶、细菌素、人富组蛋白、防卫素、杀菌肽、沃格孟汀、阿莫西林、四环素、多西环素、米诺环素、甲硝唑、新霉素、卡那霉素、克林霉素、氯化锶、硝酸钾、氟化物离子剂、薄荷油、叶绿素、利多卡因、苯佐卡因、氨基酸和过氧化物的物质。
10.一种剥离口腔软组织的方法，其包括使剥离性洁牙剂组合物接触口腔软组织，其中的洁牙剂组合物如权利要求1中的定义。
11.一种剥离口腔软组织的系统，其包含：
(A)口腔护理工具，和
(B)根据权利要求1的剥离性洁牙剂组合物。
12.权利要求11的系统，其中的口腔护理工具选自舌头清洁器、牙刷、药签、海绵、指套、棉签、牙托和磨带。
13.权利要求11的系统，其中的口腔护理工具包括其中放入剥离性洁牙剂组合物的贮库。
14.权利要求11的系统，其中的口腔护理工具包括选自塑料、树脂、木材、织物、聚合物、海绵、纸、箔、薄膜、金属和橡胶的材料。
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| PCT/US2009/039319 WO2010114549A1 (en) | 2009-04-02 | 2009-04-02 | Exfoliating dentifrice composition and method of use |
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| US (1) | US10518113B2 (zh) |
| EP (1) | EP2413884A1 (zh) |
| JP (1) | JP2012522779A (zh) |
| CN (1) | CN102378621A (zh) |
| AR (1) | AR076048A1 (zh) |
| AU (1) | AU2009343764B2 (zh) |
| BR (1) | BRPI0924837A2 (zh) |
| CA (1) | CA2757117C (zh) |
| MX (1) | MX2011009132A (zh) |
| RU (1) | RU2517136C2 (zh) |
| SG (1) | SG173787A1 (zh) |
| TW (1) | TWI391146B (zh) |
| WO (1) | WO2010114549A1 (zh) |
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| CN107666895A (zh) * | 2015-05-29 | 2018-02-06 | 高露洁-棕榄公司 | 具有脱敏剂的起泡洁齿剂 |
| CN109820748A (zh) * | 2019-03-25 | 2019-05-31 | 昆明蓝橙口腔医院有限责任公司 | 一种用于口腔产品的无水分基质及其应用 |
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| EP2907498A1 (en) * | 2014-02-13 | 2015-08-19 | Induchem Ag | Exfoliating cellulose beads and cosmetic uses thereof |
| CZ308891B6 (cs) * | 2014-10-01 | 2021-08-11 | Wald Pharmaceuticals s.r.o | Aplikační směs pro zvýšení účinnosti antiseptik a/nebo dezinficiens, aplikační prostředek obsahující aplikační směs, a použití této směsi |
| WO2021089143A1 (de) | 2019-11-06 | 2021-05-14 | Symrise Ag | Farbpartikel |
| CN111437216A (zh) * | 2020-04-22 | 2020-07-24 | 苏州清馨健康科技有限公司 | 一种抗敏牙膏 |
| CN115708793A (zh) * | 2020-09-23 | 2023-02-24 | 山东本真化妆品有限公司 | 一种不含有表面活性剂的可发泡的口腔护理组合物 |
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Cited By (3)
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| CN107666895A (zh) * | 2015-05-29 | 2018-02-06 | 高露洁-棕榄公司 | 具有脱敏剂的起泡洁齿剂 |
| CN109820748A (zh) * | 2019-03-25 | 2019-05-31 | 昆明蓝橙口腔医院有限责任公司 | 一种用于口腔产品的无水分基质及其应用 |
| CN109820748B (zh) * | 2019-03-25 | 2021-10-22 | 昆明蓝橙口腔医院有限责任公司 | 一种用于口腔产品的无水分基质及其应用 |
Also Published As
| Publication number | Publication date |
|---|---|
| AR076048A1 (es) | 2011-05-11 |
| TWI391146B (zh) | 2013-04-01 |
| RU2011144354A (ru) | 2013-05-10 |
| BRPI0924837A2 (pt) | 2015-08-11 |
| AU2009343764B2 (en) | 2012-07-05 |
| US10518113B2 (en) | 2019-12-31 |
| US20120034282A1 (en) | 2012-02-09 |
| EP2413884A1 (en) | 2012-02-08 |
| AU2009343764A1 (en) | 2011-09-22 |
| MX2011009132A (es) | 2011-09-15 |
| ZA201106243B (en) | 2015-10-28 |
| CA2757117C (en) | 2015-06-23 |
| CA2757117A1 (en) | 2010-10-07 |
| TW201102100A (en) | 2011-01-16 |
| JP2012522779A (ja) | 2012-09-27 |
| SG173787A1 (en) | 2011-09-29 |
| WO2010114549A1 (en) | 2010-10-07 |
| RU2517136C2 (ru) | 2014-05-27 |
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