CN1889829B - 包含聚合稳定剂的抗微生物组合物 - Google Patents
包含聚合稳定剂的抗微生物组合物 Download PDFInfo
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- CN1889829B CN1889829B CN2004800360853A CN200480036085A CN1889829B CN 1889829 B CN1889829 B CN 1889829B CN 2004800360853 A CN2004800360853 A CN 2004800360853A CN 200480036085 A CN200480036085 A CN 200480036085A CN 1889829 B CN1889829 B CN 1889829B
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- A61K31/00—Medicinal preparations containing organic active ingredients
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- A01N—PRESERVATION OF BODIES OF HUMANS OR ANIMALS OR PLANTS OR PARTS THEREOF; BIOCIDES, e.g. AS DISINFECTANTS, AS PESTICIDES OR AS HERBICIDES; PEST REPELLANTS OR ATTRACTANTS; PLANT GROWTH REGULATORS
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Abstract
包含碘化物和硫氰酸根阴离子、高碘酸以及含氮和/或磷的聚合物的抗微生物组合物。
Description
本发明涉及一种包含碘化物和硫氰酸根阴离子、高碘酸以及含氮和/或磷的聚合物的抗微生物组合物。
包含碘化物和硫氰酸根阴离子以及其它组分如过氧化物酶、过氧化物给体、D-葡萄糖或氧化还原酶的抗微生物组合物是本领域公知的,即公开于WO91/11105、WO95/26137或WO00/01237中。
作为包含碘化物和硫氰酸根阴离子的组合物的其它选择,基于高碘酸(已知为氧化剂和电子受体)的抗微生物组合物是已知的。例如,DE-A-4301277描述了通过在室温下用高碘酸或原高碘酸的0.1-5重量%水溶液处理容器的内表面2-20秒而将高碘酸和/或原高碘酸用于对储存和运输牛奶的容器灭菌。
EP-A-0726357描述了在阴离子纸浆和纸的加工流程中通过水解发酵细菌来抑制挥发性脂肪酸的产生和积累的方法,在该加工流程中监测存在的氢并且加入抗微生物剂和电子受体中的至少一种。对于存在电子受体和要求抑制微生物的情况下,建议使用(仲)高碘酸钠。
WO02/54872公开了包含碘化物和硫氰酸根阴离子以及高碘酸或其盐的混合物的液体抗微生物组合物。此外,该组合物任选包含过氧化物酶,特别是乳过氧化物酶。可以将这些组合物用作杀微生物剂,例如作为可以用于杀病毒和孢子的消毒剂。如果需要,在具体应用中,乳过氧化物酶在体系中的作用是增加体系的保存期和长期效力。
然而,酶是实现这一目标的昂贵方式。此外,由于酶的催化活性,在某些情况下使用酶可能对配制剂中的某些组分造成损害。例如过氧化物酶将会破坏过氧化氢。
因此,本发明所要解决的问题是用更便宜和更不具有破坏性的其它选择来代替酶如过氧化物酶和氧化还原酶。
意外地发现包含氮和/或磷基团的合成聚合物或共聚物适用于实现该目的。与不含有任何聚合物的溶液以及含有不含所述基团的聚合物的溶液相比,当使用该聚合物作为添加剂时保存期和长期效力得到显著增加。
因此,一方面,本发明提供一种液体抗微生物组合物,其中包含:
(1)碘化物阴离子和硫氰酸根阴离子的混合物;
(2)高碘酸或其盐;
和
(3)通过聚合下列物质得到的至少一种聚合物或共聚物:
(a)1-100重量%至少一种包含含氮和/或磷基团的单烯属不饱和单体,
(b)0-99重量%至少一种包含酸性基团(a)的单烯属不饱和共聚单体,
(c)0-99重量%至少一种其它的共聚单体,和
(d)0-5重量%交联共聚单体。
本发明的其它实施方案包括该组合物作为杀微生物剂(例如消毒剂或防腐剂)的用途,以及通过使该组合物与细菌、酵母、真菌、病毒或孢子接触而杀灭或抑制细菌、酵母、真菌、病毒或孢子的方法。
对于本发明,具体说明下列内容:
作为组分(1),本发明的抗微生物组合物包含碘化物阴离子和硫氰酸根阴离子的混合物。作为其各自的盐提供阴离子。合适的阳离子包括碱金属阳离子、铵离子、离子和碱土金属阳离子。也可以作为HI提供碘化物。优选作为K盐或Na盐提供阴离子。
在本发明实施方案的组合物中,碘化物∶硫氰酸根阴离子的重量比优选为0.1∶1到50∶1,更优选为0.2∶1到20∶1,最优选为1∶1到3∶1,包括端点。
作为组分(2),该抗微生物组合物包含高碘酸或其盐。
高碘酸[CAS RN 10450-60-9],有时指原高碘酸,具有下式:
在高碘酸盐中合适的阳离子包括碱金属离子如Li+、Na+或K+,碱土金属离子如Mg2+或Co2+,铵和烷基铵阳离子如NH3R+、NH2R2 +、NHR3 +和NR4 +,其中R独立地代表有机基团,优选C1-C10烷基或芳烷基。
作为组分(3),该抗微生物组合物包含上述聚合物或共聚物。
合适的具有含氮基团的单烯属不饱和单体(a)的例子包括含氮丙烯酸衍生物如丙烯酰胺、N-取代的H-丙烯酰胺,或者含氮丙烯酸酯如甲基丙烯酸二甲氨基乙酯,N-乙烯基酰胺如N-乙烯基甲酰胺、N-乙烯基-N-甲基甲酰胺、N-乙烯基乙酰胺、N-乙烯基-N-甲基乙酰胺、N-乙烯基-N-甲基丙酰胺和N-乙烯基丙酰胺。其它的合适单体为N-乙烯基咪唑和在内酰胺环中含有5-13个碳原子的N-乙烯基内酰胺。例子包括N-乙烯基吡咯烷酮、N-乙烯基丁内酰胺、N-乙烯基己内酰胺、N-乙烯基戊内酰胺和N-乙烯基月桂内酰胺。
也可以在聚合后对单体单元改性。如果含氮基团可水解,那么可以将该基团水解。
具有含磷基团的合适单体的例子包括乙烯基膦酸酯。
将这些单体(a)中的至少一种用作组分,即所得聚合物可以是均聚物。然而,优选该聚合物是由至少两种不同单体(a)或者由至少一种单体(a)和至少一种其它单体(b)和/或(c)组成的共聚物。
两种单体(a)的优选组合包括乙烯基咪唑和N-乙烯基吡咯烷酮。
相对于聚合物的总重量,单体(a)在聚合物中的量为1-100重量%。优选该量为5-100重量%,更优选10-60重量%,最优选15-50重量%。
共聚单体(b)包含至少一个酸性基团或其衍生物如盐或酸酐。酸性基团的例子包括-COOH基团、亚磷酸基团、膦酸基团或磺酸基团。
合适共聚单体(b)的例子包括丙烯酸、甲基丙烯酸、马来酸、富马酸、乙烯基磺酸、乙烯基膦酸或亚磷酸单乙烯基酯或亚磷酸单烯丙酯。
优选的单体(b)是丙烯酸、甲基丙烯酸和马来酸。共聚单体(b)的存在量可以为0-99%。优选存在量为0-95%,更优选20-70%,最优选25-65%。
可以使用两种不同类型的共聚单体(c)。一类包括不同于(a)和(b)的单烯属不饱和单体,即不包含含氮或磷基团或酸性基团,但是可通过相同的聚合技术与(a)和(b)共聚的单烯属不饱和单体。
合适的例子包括烯烃如乙烯或丙烯,乙烯基芳族单体如苯乙烯,乙烯醇或其酯如乙酸乙烯酯或丙酸乙烯酯,或者丙烯酸或甲基丙烯酸的酯。
第二类共聚单体(c)不包含烯属不饱和基团,并且该共聚单体不能通过相同的聚合技术与单体(a)和(b)共聚。该共聚单体(c)的例子包括适合形成聚醚的单体,特别是烯化氧如环氧乙烷、环氧丙烷或环氧丁烷,1,ω-二醇如乙二醇、1,3-丙二醇、1,4-丁二醇,或环醚如四氢呋喃(THF)。
优选的共聚单体(c)包括环氧乙烷、环氧丙烷、乙二醇、1,3-丙二醇和1,4-丁二醇。
共聚单体(c)的存在量可以为0-99%,优选为0-75%,更优选为20-70%,最优选为20-60%。
可以通过本领域技术人员已知的任何聚合技术制备所述单体的聚合物和共聚物。优选通过组分(a)、任选的(b)以及任选的第一类单体(c)的自由基聚合而进行聚合。可以在溶液、分散体、悬浮液、乳液或本体中进行聚合。合适的条件是本领域技术人员已知的。
如果使用第二类单体(c),则必须使用两种不同的聚合技术。首先使用所述单体(c)以形成聚醚,例如通过阳离子聚合或者通过缩聚。优选的聚醚是聚环氧乙烷。第二步,在聚醚存在下通过自由基聚合使单体(a)和任选的(b)发生聚合。在这些条件下,形成接枝聚合物。该技术的详情例如公开于EP-A 1136254及其中引用的文献中。当然,单体(a)和任选的(b)的链段以及单体(c)的链段也可以通过本领域技术人员已知的其它技术相互连接。
作为化合物(d),该聚合物可以另外包含交联剂;然而,应当避免过度交联。如果存在的话,交联剂的量应当不高于5重量%,优选不高于3%,最优选不高于2%。合适交联剂的例子包含具有两个或更多个非共轭烯属不饱和基团的单体,例如丁二醇二(甲基)丙烯酸酯或己二醇二(甲基)丙烯酸酯。
本领域的技术人员可以通过选择单体(a)和任选的(b)和/或(c)和/或(d)的量和性质而改变本发明使用的聚合物的性质。可以得到水溶性聚合物或油溶性聚合物。
对于本发明而言,优选使用可溶于或至少可分散于水中的聚合物。
本发明的抗微生物组合物可以直接使用或者通过组合/混合各组分的单独溶液而使用。可以将该组合物直接加入(优选在各组分相互剧烈混合后)待保护的介质中。
然而,优选将组合物配制成糊剂、乳剂、溶液或施加在固体载体上。
优选该组合物为液体组合物,并且优选该组合物含有水。
含有水的组合物可以是所有组分在合适的溶剂混合物中的溶液。合适的溶剂混合物优选包含至少50重量%的水,更优选包含至少80%的水,最优选溶剂仅为水。溶剂混合物中的其它组分可以是与水混溶的有机溶剂。合适组分的例子包含一元醇如甲醇、乙醇、1-丙醇或2-丙醇,二元醇如乙二醇或1,4-丁二醇,以及聚醚醇如二甘醇。
该组合物还可以另外含有表面活性剂或乳化剂,以使该组合物为水包油型乳液或基于表面活性剂的溶液。
该组合物还可以含有其它添加剂和助剂,例如染料、缓蚀剂、盐、香料、消泡剂、表面活性剂、乳化剂或螯合剂。
该组合物可以与其它活性剂结合使用,其它活性剂例如为己二酸、苯甲酸、联苯基-2-酚、溴硝丙二醇(bronopol)、次氯酸钙、十六烷基氯化吡啶、氯甲酚、氯二甲酚、D-葡糖酸和N,N”-二(4-氯苯基)-3,12-二亚氨基-2,4,11,13-四氮杂十四烷二脒(2∶1)的化合物、2,2-二溴-2-氰基乙酰胺、乙醇、甲醛、甲酸、戊二醛、2,4-己二烯酸、过氧化氢、碘、1-苯氧基-2-丙醇和2-苯氧基丙醇、L-(+)-乳酸、低聚-(2-(2-乙氧基)乙氧基乙基氯化胍)、五钾二(过一硫酸盐)二(硫酸盐)、过乙酸、2-苯氧基乙醇、邻苯二甲醛、6-(邻苯二甲酰亚氨基)过氧己酸、聚(六亚甲基二胺氯化胍)、(E,E)-2,4-己二烯酸钾、1-丙醇、2-丙醇、季铵化合物(例如苄基-烷基二甲基氯化铵、[2-[[2-[(2-羧乙基)(2-羟乙基)氨基]乙基]氨基]-2-氧代乙基]椰油烷基二甲基氢氧化铵、苄基-C12-14烷基二甲基氯化铵、苄基-C12-16烷基二甲基氯化铵、苄基-C12-18烷基二甲基氯化铵、C12-14烷基[(乙基苯基)甲基]二甲基氯化铵、n-C10-16烷基三亚甲基二胺和氯乙酸的反应产物、二C8-10烷基二甲基氯化铵、二烷基(C8-18)二甲基铵化合物、二癸基二甲基氯化铵、十六烷基氯化吡啶、谷氨酸和N-(C12-14烷基)丙二胺的反应产物)、水杨酸、氯化银或其它银盐、2-联苯酚钠、二氯异氰脲酸钠二水合物、二氯-异三聚氰酸钠(sodiumdichloro-s-triazinetrione)、次氯酸钠、对氯间甲酚钠、氯胺T钠(sodiumtosylchloramide)。
优选的可联用产品为氯甲酚、氯二甲酚、乙醇、甲醛、甲酸、戊二醛、过氧化氢、1-苯氧基-2-丙醇和2-苯氧基丙醇、2-苯氧基乙醇、邻苯二甲醛、聚六亚甲基双胍、1-丙醇、2-丙醇或上述季铵化合物。
本发明实施方案的组合物可以作为抗微生物剂,例如作为防腐剂或作为消毒剂。
特别是,本发明实施方案的组合物在抵抗细菌、酵母、真菌、病毒和孢子如杆菌孢子时特别有效。
典型应用浓度为:
组分 | 典型浓度 | 优选 |
高碘酸或其盐 | 0.01-100mmol/l | 0.05-10mmol/l |
碘化物离子 | 0.005-50mmol/l | 0.05-10mmol/l |
硫氰酸根离子 | 0.005-50mmol/l | 0.05-10mmol/l |
(共)聚合物 | 0.005-10重量% | 0.1-5重量% |
当然也可以作为浓缩物配制组合物并在使用前将其稀释。各组分可以配制成单独的浓缩物。以同样的方式,可以将浓缩物或组分浓缩物加入待保护的介质中以达到上述浓度。
该组合物的pH值可以为1-8,但优选小于6.0,特别是在低pH值下,该组合物可以包含游离的高碘酸。然而,该组合物可作为其它选择而包含或额外包含碱金属,特别是钠及其盐。可以使用合适的缓冲体系调节pH值。
可以使用该组合物的应用领域是:皮肤消毒剂,抗微生物皂,晒黑剂,医疗设备的消毒,游泳池等的处理,空气调节加工,人类居所的卫生,化学盥洗用品,污水/废水处理,医院传染性废水和污物或其他物质的处理,洗衣,动物的窝/棚/机器/鞋袜、孵化器、运输设备的消毒,鱼类养殖,食品加工厂的地板、墙壁和设备,无菌包装材料的制造。
除了将组合物用作抗微生物剂(例如作为上述的防腐剂或消毒剂)之外,本发明实施方案的抗微生物组合物可以在要求有效抗病毒、抗菌、抗霉菌和/或抗酵母活性的各种产品中提供活性组分。这类产品的例子包括:
(a)除臭剂,例如以洗液的形式局部给药;
(b)抗菌皮肤洗涤液,例如以洗剂形式;
(c)抗痤疮制剂,例如以洗剂或乳膏形式;
(d)抗足癣制剂,例如以洗剂形式;
(e)去头屑制剂,例如以香波或洗剂形式;
(f)牙科制剂,例如适合一般口腔卫生的漱口剂,特别是具有抗牙菌斑性质的那些,以及洁齿剂如牙膏、口香糖和糖锭;
(g)浸渍材料,例如伤口包扎材料、缝合线和牙线;
(h)药物,例如伤口冲洗剂和灼伤治疗剂、抗腹泻剂以及适合治疗传染病如假丝酵母和癣菌传染病的药物;
(i)眼科制剂,例如洗眼剂和/或隐形眼镜消毒液;和
(j)杀菌剂,例如用于乳瓶和外科或牙科器械。
另一方面,本发明提供了一种杀灭或抑制病毒或孢子的方法,该方法包含使上述组合物与病毒或孢子接触。
可以通过处理待保护的目标而使用本发明实施方案的组合物,例如用该组合物处理医疗设备等。这例如可以通过将目标浸入溶液或将溶液喷雾到目标上来完成。
此外,可以将该组合物加入待保护的介质中。在后者的情况下,可以使用所有组分的溶液,然而当然也可以单独加入各组分;即,盐溶液和聚合物溶液。对于本发明的范围,仅需要所有组分都存在于待保护的介质中。
现在参考下列实施例更详细描述本发明实施方案。
实施例
对于所有的实施例和对比例,使用NaSCN、NaI和高碘酸的水溶液(pH值3.8)。
所有样品的浓度为:0.9mmol/l高碘酸盐、0.4mmol/l碘化物和0.6mmol/l硫氰酸盐。
以表1所示的浓度将聚合物加入每一个所述溶液中。为了对比,其中一个样品中没有加入任何聚合物。
通过将所有的组分溶解于水中得到要求的浓度而制备表1中总结的样品。将溶液储存在室温下,并且在表1所述的储存时间点进行试验。测试程序包含对储存溶液取样,并且用表1所述的生物体进行接种。如果与溶液接触5分钟后显示生物体减少5个对数值,那么溶液符合阳性结果的测试标准。
所有实验总结在表1中。
备注+有效。混合物在储存一个月后,黑曲霉和大肠杆菌在5分钟内减少至少5个对数值
-无效。混合物在储存一个月后,黑曲霉和大肠杆菌在5分钟内减少小于5个对数值
实施例和对比例清楚地说明了使用包含含N或P基团的聚合物显著提高了稳定性和长期活性。不含所述基团的聚合物没有表现出这样的效果。
Claims (7)
1.一种抗微生物组合物,其中包含:
(1)0.005-50mmol/l的碘化物阴离子和0.005-50mmol/l的硫氰酸根阴离子的混合物,其中碘化物阴离子与硫氰酸根阴离子的重量比为0.2∶1到20∶1,
(2)0.01-100mmol/l的高碘酸或其盐,和
(3)0.005-10重量%的至少一种含有下列单元的聚合物或共聚物
(a)5-100重量%至少一种包含含氮基团的单烯属不饱和单体,该单体选自:含氮丙烯酸衍生物,N-乙烯基酰胺,N-乙烯基咪唑和在内酰胺环中含有5-13个碳原子的N-乙烯基内酰胺,
(b)0-95重量%至少一种包含酸性基团的单烯属不饱和共聚单体,该单体选自:丙烯酸、甲基丙烯酸、马来酸、富马酸、乙烯基磺酸、乙烯基膦酸、亚磷酸单乙烯基酯或亚磷酸单烯丙酯,
(c)0-75重量%至少一种选自如下的共聚单体,
-不同于(a)和(b)的单烯属不饱和单体,和
-适合形成聚醚的不包含烯属不饱和基团的单体,
和
(d)0-5重量%的包含两个或更多个非共轭烯属不饱和基团的交联共聚单体。
2.根据权利要求1的组合物,其中共聚物单元的量为:
(a)10-60%,
(b)20-70%,
(c)0-70%,和
(d)0-5%。
3.根据权利要求1或2的组合物,其中该组合物为液体组合物。
4.根据权利要求3的组合物,其中该组合物的溶剂包含水。
5.根据权利要求1的组合物,其中所述共聚物包含乙烯基咪唑和N-乙烯基吡咯烷酮作为单体(a)。
6.根据权利要求1-5中任一项的组合物作为皮肤消毒剂,抗微生物皂,晒黑剂,医疗设备的消毒,游泳池的处理,空气调节加工,人类居所的卫生,化学盥洗用品,污水、废水处理,医院传染性废水和污物的处理,洗衣,动物的窝、棚、鞋袜、孵化器、运输设备的消毒,鱼类养殖,食品加工厂的地板、墙壁和设备,或无菌包装材料的制造用杀微生物剂的用途。
7.根据权利要求1-5中任一项的组合物作为除臭剂,抗菌皮肤洗涤液,抗痤疮制剂,抗足癣制剂或去头屑制剂中的活性组分的用途。
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