CN101076322A - 用于动植物收获前后处理的抗微生物组合物 - Google Patents
用于动植物收获前后处理的抗微生物组合物 Download PDFInfo
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Abstract
本发明提供了一种抗微生物、抗菌工艺助剂，食物添加剂和食物组分以抑止已知的病原体、指示菌和腐败生物体如沙门氏菌、葡萄球菌、李斯特氏菌、大肠杆菌等。本发明的抗微生物试剂用于动物饲料处理、食物收获前后的处理、空气传播污染的熟食处理及其它需要杀菌和消毒的条件。所述的抗微生物试剂的一个主要优点是抑止具有抗生素抗性的细菌的生长。
Description
本发明要求2004年2月26日递交的美国临时申请序号60/547,991的优先权。
技术领域
本发明涉及一种抗菌剂，特别是一种组合物，一种制备和使用该组合物用于抗微生物、抗细菌和食物收获前后处理以抑止已知的污染人类食物链的病原体、指示菌和腐败生物体的生长。
背景技术
在人类食物链中的蛋白质源，如蛋、生肉、家禽、猎禽、牛奶和乳制品、鱼、虾、蛙腿等，带来潜在的营养和潜在的疾病和死亡。人类饮食中的可食用植物，如水果、蔬菜、谷物在污染的环境中收获和处理也会带来潜在的疾病和死亡。熟知的病原体，如沙门氏菌、李斯特氏菌和大肠杆菌，以及指示菌(indicator)和腐败生物体包括葡萄球菌，能够在人类消费的生肉、水果和蔬菜或者半熟食或熟食、动物制品的处理或者收获之前或过程中发现。
商业、旅游和通讯的全球化带来了对设区和国家之间全球范围内的交换，包括潜在的细菌生态***的全球化关注的提高。在二十世纪四十年代中期，有害细菌曾经用抗生素如青霉酸控制过；但是，当抗生素抗性细菌在全球范围内越来越多时，这种控制就不再存在了。例如，在1946年以前，大约90％在医院分离的葡萄球菌奥里斯对青霉酸敏感，到了1952年，分离的75％的是青霉酸抗性。作为对人和兽药的主要威胁，细菌对抗微生物试剂的抗性遍及全世界。对抗生素和抗微生物试剂的抗性以惊人的速率出现的原因有多种，如群集和拥挤过度，抗生素在动物培养和水产业的使用，老龄人数的增长，旅游的发展，抗生素的滥卖，抗生素自我治疗，感染控制资源的匮乏，以及抗生素的不当使用。
因此，世界人口面临获得抗微生物抗性的食物和水源传染危险升高。即使在最重要的病原体细菌中普遍存在的抗性的微小提高也会导致治疗失败和其它不利后果包括死亡可能性的增加。
在人体和可食用动物中适当的使用抗微生物试剂对于维持抗微生物有效性和减少抗性生物发展的可能性是必要的。虽然在可食用动物中治疗使用抗微生物试剂对于提高动物健康和提供可消费的肉、奶和蛋是重要的，但关键是保持抗微生物试剂在人类药品中的长期效果。本发明提供一种没有已知的毒性和抗性并能用于保护公众健康的抗微生物试剂加工助剂和食物添加剂。
在授予Cummins的5,989,595和6,242,011B1号美国专利中，公开了一种用于杀死腐败食物如鱼的微生物的酸性组合物。Cummins取得专利的该组合物还对治疗皮肤的黑素瘤和其它病原体有用，并作为本发明的新的抗微生物试剂的前体。
授予Brinton等的美国专利5,997,911教导了一种能够溶解于饮用水的简单铜盐、羟基羧酸和缓冲剂如铵盐，以有效剂量用于火鸡和猪止泻药。
授予Hei等的美国专利6,506,737B1公开了一种食品工业用抗微生物组合物，包括硫酸、硫酸盐和卤化铵盐，提供一种在其他应用中进行表面清洁和消毒的凝胶状化合物。卤化物成分的使用限制了人或者动物的吸收用途，并且对机械、植物和其它植被有害。
授予Jones等的美国专利6,565,893B1描述了一种用于游泳池等水性消毒剂，其中五水硫酸铜、水、硫酸和硫酸铵在“冷加工法”中结合，该配方保持在40℉以上以保持金属离子悬浮。
授予Cook等的美国专利公开号为2003/0118705A1描述了一种可吸收消毒剂，其可消除和控制植物、动物、人类、植物和动物制品以及感染病原体的物品的病原体；该消毒剂包括硫酸、水和金属离子，特别是铜、银和金。
总体而言，上述文献没有提供不含卤素的组合物，其在较宽温度和pH范围内稳定，可吸收，并且对人类和其它动物消费的食物收获前后的处理都有效。本发明的组合物在无数收获前后的应用上安全有效，并且对环境安全。
发明内容
本发明的第一个目的是提供一种抑止病源性生物体细胞生长的组合物及其制备方法。
本发明的第二个目的是提供一种抑止指示菌和腐败生物体细胞生长的组合物及其制备方法。
本发明的第三个目的是提供一种用于热烫池水浸泡禽类和其他动物畜体的组合物及其制备方法。
本发明的第四个目的是提供一种用于肉类生产线，包括但不限于喷淋、最后冲洗和激冷水池中水处理工艺的组合物及其制备方法。
本发明的第五个目的是提供一种用于废水处理的组合物及其制备方法。
本发明的第六个目的是提供一种用于动物饲料和水处理的组合物及其制备方法。
本发明的第七个目的是提供一种用于抗人类、植物和动物疾病以及在收获前或后植物和植物表面最小化疾病生长和传播的组合物及其制备方法。
本发明的第八个目的是提供一种用作医院、家庭和其它确实需要硬表面杀菌区域的表面杀菌剂的组合物。
本发明的第九个目的是提供一种抑止具有抗生素抗性的病原体、指示菌和腐败生物体的组合物。
本发明的第十个目的是提供一种用于制冰机的组合物，以便用在食物收获后的处理工艺并具有额外的抗微生物功能。
本发明的另一个目的是提供一种抗微生物助剂，用于减少食物如奶、禽类、蛋、红肉、猪肉和海产品收获前或收获后、处理后过程中或处理后的微生物污染。
本发明的其它目的和优点，通过优选实施方式并结合表格和附图说明，更加详细说明而显而易见。
附图说明
图1是图表，示出了PHB0020在病原体和腐败菌隔离暴露2分钟的效果。
图2是图表，示出了菌落对数水平的减少。
具体实施方式
在详细解释本发明的实施方式之前，应该理解本发明的应用不限于示出的特定安排的细节，因为本发明能够用其它实施方式实现。此外，本文使用的术语的目的是描述而不是限定。
在讨论组合物和其制备方法之前，讨论本文中使用的某些词语的含义和应用是有益的：
收获前—本文中的含义为动植物在出生或者种子发芽之后、停止生长和结束生命之前的任何时间。
收获后—指的是动植物停止生长和结束生命之后的任何时间，包括非食物涉及处理和制备食物的硬表面。
PHB0020—五水硫酸铜和/或其它形式的铜离子，硫酸银和/或其它形式的银离子，加入到pHarlo用于本发明的抗微生物、抗菌添加剂。
PHB0028—作为动物饲料添加剂的配方。
PHB0128—用作废水处理添加剂的配方。
pHarlo—授予Cummins的美国专利5,989,595和6,242,001B1中要求保护的组合物，引入本文作为参考并将在下文中详细描述。
E-coli—大肠杆菌，指示菌
李斯特氏菌—单核细胞增多性李氏菌，一种病原体
假单胞菌—荧光假单胞菌，腐败菌
沙门氏菌—鼠伤寒沙门氏菌，一种病原体
希瓦氏菌—腐败希瓦氏菌，腐败菌
葡萄球菌—金黄色葡萄球菌，一种病原体
本发明酸性组合物及其制备方法与美国专利5,989,595和6,242,001B1中描述的相似，引入本文作为参考。
首先，选择一带有冷却套管且没有电极装置的压力容器；但是，所优选的压力容器配备有两个电极，一个阳极一个阴极，以在容器底部上方1英尺处提供直流电(DC)。所述电极距离约三(3)英尺。
本发明的工艺步骤包括将纯度约94％-99.9％的硫酸以1-2的容积比例与蒸馏水和硫酸铵结合提供混合物(I)，蒸馏水和硫酸铵的比例为2.77磅硫酸铵每加仑蒸馏水。混合物(I)在带有两个预先放置的电极，一个阳极一个阴极的压力容器中结合。在加入硫酸铵的过程中，向混合物加直流电(DC)。直流电的强度范围为约1安培-100安培，优选约1安培-5安培。然后将混合物在约高于大气压1-15磅每平方英寸(psi)的压力下加热。在约200℉-1200℉的范围内加热混合物，优选约800℉-900℉大约30分钟。在上述特定的压力和温度下，本领域的熟练技术人员应该理解，明智的选择温度、时间和压力是需要的，并且应该调整以维持安全的化学反应。
冷却混合物之后，加入稳定剂。在加热之前该稳定剂是混合物(I)的一部分。稳定剂的用量约为混合物(I)总重量的10％重量。所得的酸性组合物的pH值为负三(-3)，对于消灭微生物有用。本发明的创造性步骤需要加入含有金属离子的化合物以扩大本文讨论的抗微生物特性。未稀释时得到以下物理和化学特性。
pH＝-3，由非酸性氢质子计数，该数据经各种电极类型误差校正，由EFE&H分析机构执行，EPA(美国环保署)认可的实验室。
溶液中金属离子的稳定性：pH值约从0至9
金属离子的温度稳定性：约从32℉至蒸发温度或者约212℉。
各种其它带有金属离子的化合物可以替代五水硫酸铜。以下金属盐适宜于替代：
硫酸铜、谷氨酸铜、氧化锌、谷氨酸锌、谷氨酸镁、硫酸镁、硫酸银、氧化银及其混合物。
对于pHarlo Blue 0020，以下称作PHB0020，它是一种抗微生物、抗菌剂，其配方通常被美国食品及药品管理局承认是安全的(GRAS)。PHB0020对于收获前后的食品资源以及食品，包括但不限于植物、水果、蔬菜、蛋、禽类、海产品、肉和动物及猪肉制品的处理有用。组合物如下表A所列：
表A
| 组分 | 百分数 |
| 五水硫酸铜 | 16.4 |
| 硫酸(加工助剂) | 9.9 |
| 硫酸铵 | 2.2 |
| 蒸馏水 | 71.5 |
所述组分形成浓缩液，以少于0.10毫升(ml)的极少量与1加仑水结合形成PHB0020。
以下的实施例、图和表提供PHB0020作为抗微生物试剂和食品添加剂更具体的应用和效果。
实施例1
在禽类和动物产品的加工厂，通常使用各种水处理工艺，如热烫池、喷淋槽、最后冲洗及激冷水池。热烫池用于在禽类褪毛之前浸泡；其它动物浸泡以除去外层覆盖的毛发。热烫处理允许交叉污染和传播病原体。重要的是为了人类食品供应安全提供可在水处理中使用的添加剂，以抑止病原体和有害细菌的成长和传播。理想的添加剂在沸点温度不蒸发，不被高温破坏，且不被有机物束缚，如血和粪以及无用的动物油脂。
PHB0020在病原体、指示菌和在用家禽热烫水鸡体锅炉相关的腐败菌种群的效果在本发明的一个实施例种确定。
首先，从商业禽类热烫机的溢流或者进口端收集热烫水。将水杀菌或者热压处理以消除所有群落的细菌和细菌孢子以避免在研究过程中干扰。热压热烫机水进行化学评价并与原来的热烫机水对比以保证所需的生和热压热烫机水有机物质相似。
其次，准备多组试管通过加入9毫升(ml)杀菌热烫水的给聚苯乙烯试管杀菌。加入9毫升杀菌热烫水的一组作为控制组。一组加入杀菌热烫水和PHB0020(消毒剂)直到pH值为2.2。
各菌种均暴露于约130℉(55℃)带有PHB0020消毒剂的杀菌热烫水约两分钟以模拟热烫。
在暴露之后，例如可以利用有氧板计数法通过倾倒平板1毫升悬浮液，并在95℉(35℃)培养48小时。
下表I记录了在热烫水方案中微生物生长结果，其中杀菌水加热到热烫温度，范围约为120℉(490C)至140℉(60℃)热烫温度，优选到约130℉(55℃)。加入各种浓度的PHB0020，范围在约0.4/1ppm(parts per million)至约0.8ppm，优选约0.6ppm，病原体、指示菌和腐败菌菌落暴露于经处理的热烫水。
表I—热烫水方案
细菌：鼠伤寒沙门氏菌
对照例
| 暴露样本编号： | 群落形成细菌单元 | 对数减少 | 热烫水处理之后的生长 |
| 水123456789 | 4308809704506207001140620580 | 2.6334682.9444832.9867722.6532132.7923922.8450983.0569052.7923922.763428 | 阴性(无生长)阴性阴性阴性阴性阴性阴性阴性阴性 |
细菌：金黄色葡萄球菌
对照例
| 暴露样本编号： | 群落形成细菌单元 | 对数减少 | 热烫水处理之后的生长 |
| 水12生长345678生长9 | 530550580500540420530480470 | 2.7242762.7403632.7634282.6989702.7323942.6232492.7242762.6812412.672098 | 阴性(无生长)一(1)菌落阴性阴性阴性阴性阴性一(1)菌落阴性 |
细菌：荧光假单胞菌
对照例
| 暴露样本编号： | 群落形成细菌单元 | 对数减少 | 热烫水处理之后的生长 |
| 水123456生长789 | 5408807906201120790520013601040 | 2.732342.9444832.8976272.7923923.0492182.8976273.7160033.1335393.017033 | 阴性阴性阴性阴性阴性一(1)菌落阴性阴性阴性 |
细菌：单核细胞增多性李氏菌
对照例
| 暴露样本编号： | 群落形成细菌单元 | 对数减少 | 热烫水处理之后的生长 |
| 水1生长2生长34生长5生长6789 | 172018401440182014401880172017201740 | 3.2355283.2648183.1583623.2600713.1583623.2741583.2355283.2355283.240549 | 五(5)菌落六(6)菌落阴性(五无生长)五(5)菌落一(1)菌落阴性阴性阴性阴性 |
细菌：腐败希瓦氏菌
对照例
| 暴露样本编号： | 群落形成细菌单元 | 对数减少 | 热烫水处理之后的生长 |
| 水123456789 | 505060205070802030 | 1.6989701.6989701.7780511.3010301.6989701.8450981.9030901.3010301.477121 | 阴性(无生长)阴性阴性阴性阴性阴性阴性阴性阴性 |
细菌：大肠杆菌
对照例
| 暴露样本编号： | 群落形成细菌单元 | 对数减少 | 热烫水处理之后的生长 |
| 水1234生长5生长6789 | 15100000129000001330000012200000134000001220000014200000136000007600000 | 7.1789777.1105907.1238527.0863607.1271057.0863607.1522887.1335396.880814 | 460菌落生长阴性(无生长)32菌落生长1170菌落4700菌落57菌落生长900菌落生长410菌落生长37菌落生长 |
参考图1，该图表示出了由上表鉴定PHB0020在病原体和腐败菌的效果。该图表分为两部分，左边是对照例示出了各菌种菌落形成单位的对数，右边是各菌种在暴露于经PHB0020处理的热烫水两分钟的菌落形成单位。该图表示出了李斯特氏菌，一种革兰式阳性菌，很难被杀死，和增殖能力很强的大肠杆菌在2分钟暴露后减少最多。
在图表2中示出了各菌种细菌水平的对数减少。在绝大多数情况下，群落形成单元少于三，增殖最强的大肠杆菌的对数少于五。
因此，PHB0020具有抗微生物试剂、杀菌剂或者消毒剂的作用，并且在工业热烫条件下极其有效地消除商业热烫水中的病原体、指示菌和腐败菌。PHB0020是一种控制热烫水中细菌的有效方式并且可以用于控制热烫过程中的交叉污染。家禽热烫水杀菌是极其重要的因为它是工厂中禽类首先浸入的普通浴槽，并且细菌可以在禽类之间传播。
作为抗微生物试剂的PHB0020的效果适宜于许多其它用途和一定量的范围，在下表J中标识：
表J
使用水平毫克每升(mg/L)
| PHB0020的应用：收获前 | 范围 | 目标 |
| 孵化场 | 1.0-2.0mg/L | 1.3mg/L |
| 洗蛋 | 0.8-1.5mg/L | 1.0mg/L |
| 家畜饮用水 | 0.8-2.0mg/L | 1.2mg/L |
| 动物饲料 | 0.6-2.0mg/L | 1.0mg/L |
| 海产品水供应*** | 0.4-1.5mg/L | 0.8mg/L(依据类型) |
| 动物脚杀菌 | 约1-50mg/L | 约20mg/L |
| 收获后 | ||
| 禽类：(小鸡、火鸡、猎禽、鸵鸟、鸭子、鹅、野鸡) | ||
| 1.热烫机 | 0.4-0.8至3mg/L | 依据化学用水 |
| 2.激冷水槽 | 0.6-1.0mg/L | 0.8mg/L |
| 3.最后冲洗 | 0.4-0.8mg/L | 0.6mg/L |
| 红肉 | 0.8-1.2mg/L | 1.0mg/L |
| 海产品(鱼、贝、蛙、章鱼、鱿鱼) | 0.4-1.0mg/L | 0.8mg/L |
| 废水 | 0.6-1.0mg/L | 0.8mg/L |
| 熟食空气传播污染 | 0.4-1.0mg/L | 0.8mg/L |
| 防腐涂层 | 0.4-0.8mg/L | 0.6mg/L |
| 冰产品成分 | 0.6-1.0mg/L | 0.8mg/L |
上表标识了本发明的某些应用；它是这种0.4-0.8新的可用于保护公众健康的抗微生物组合物无数潜在商业用途的指示。
本发明的组合物的收获前和非食品应用将进一步详细讨论。所述组合物通过稀释水稀释可以制成多种形式，如气雾剂、细雾、蒸汽或雾以制备能够在空气中悬浮一段时间的微米粒子，并作用于与其接触的空气传播的病原体。本发明的组合物能够除去孵化场的氨水味，改进动物供水***，和能够用于洗涤液涂层以及其它杀菌食物在收获前，如孵化场、乳制品和洗蛋。其它用途有乳牛的口腔护理和作为洗脚或者杀菌。可以预期，本发明组合物的许多非食品应用包括，有效控制微生物或者病原体种群，如食品制备设备、器具、计数器顶层、传送带、脚手冲浸槽、储存设施、空气循环***、冷却器、热烫机、墙和底板等。
具体的动植物收获后处理包括但不限于，植物、水果、蔬菜、动物副产品、鱼和贝的水处理。所述处理包括冲洗、浸渍和清洗食品，本发明的组合物在热烫池、冲洗和喷雾射流及激冷器有效。其最终结果是人类和其它动物的安全、健康的食品供应。
虽然本发明已经以实践中假定的特定实施方式或者变形的不同的术语描述、公开、示例和示出，本发明的范围既不被打算，也不被认为限于此，其它此类如通过本发明的教导的变形或实施方式特别是落入所附的权利要求书范围内的被特别保留。
Claims (26)
1.一种用于食物收获前和收获后处理的产品，以抑止已知的病原体、指示菌和腐败菌的细胞生长，由以下工艺制备：
(a)将纯度约94％-99.9％的硫酸以1-2的容积比例与蒸馏水和硫酸铵结合提供混合物(I)，蒸馏水和硫酸铵的比为2.77磅硫酸铵每加仑蒸馏水；
(b)然后在高于大气压的压力容器中处理混合物(I)并将混合物加热到约200-1200至少30分钟；
(c)冷却混合物；
(d)加入稳定剂，该稳定剂是混合物(I)的一部分，并占约混合物(I)总重量的10％重量，并由此形成混合物(II)；然后
(e)向混合物(II)中加入含有金属离子的化合物形成混合物(III)。
2.权利要求1的工艺制备的产品，其中的金属离子选自由铜离子、银离子、锌离子、镁离子及其混合物组成的组。
3.权利要求1的工艺制备的产品，其中含有金属离子的化合物是至少选自硫酸铜、五水硫酸铜、谷氨酸铜、氧化锌、谷氨酸锌、谷氨酸镁、硫酸镁、氧化银和硫酸银中的一种。
4.权利要求1的工艺制备的产品，进一步包括在添加硫酸铵的过程中向混合物(I)应用直流电(DC)的步骤。
5.权利要求4的工艺制备的产品，其中DC电的范围约为1-100安培。
6.权利要求5的工艺制备的产品，其中DC电的范围约为1-5安培。
7.权利要求3的工艺制备的产品，其中含有金属离子的化合物与蒸馏水结合形成溶液。
8.权利要求4的工艺制备的产品，其中所述化合物的蒸馏水溶液含有金属离子的量占混合物(III)总重量的范围约为2％-75％重量。
9.权利要求1的工艺制备的产品，用于抑止细胞增长的病原体选自由鼠伤寒沙门氏菌、单核细胞增多性李氏菌、荧光假单胞菌组成的组。
10.权利要求1的工艺制备的产品，抑止生长的指示菌是大肠杆菌。
11.权利要求1的工艺制备的产品，抑止生长的腐败菌至少选自以下一种：荧光假单胞菌和腐败希瓦氏菌。
12.权利要求1的工艺制备的产品，用作浸泡禽类的加工生产线中热烫池水的添加剂。
13.权利要求1的工艺制备的产品，用作生肉水处理工艺的添加剂，所述的处理工艺选自以下一种：热烫、喷淋、最后冲洗及激冷水。
14.权利要求1的工艺制备的产品，用作废水处理的添加剂。
15.权利要求1的工艺制备的产品，用作以下至少一种的洗涤用水：蛋、水果和蔬菜。
16.权利要求1的工艺制备的产品，用作动物饲料添加剂。
17.权利要求1的工艺制备的产品，用作禽类饲料添加剂。
18.权利要求1的工艺制备的产品，用作冰产品的添加剂。
19.权利要求1的工艺制备的产品，用作抗微生物助剂以减少食物微生物污染，所述食物至少选自以下一种：禽类、红肉、猪肉、鹿肉、海产品、蛋、牛奶和乳制品。
20.权利要求1的工艺制备的产品，用于乳牛脚的洗涤和杀菌。
21.一种用于收获前和收获后的食物和非食物处理的抗微生物混合物的制备方法，包括步骤：
(a)向第一容器中加入纯度约94％的硫酸；
(b)在一个独立容器中加热两倍于硫酸体积的蒸馏水至至少140；
(c)在热水中以2.77磅每加仑水的比例结合硫酸铵形成混合物(I)；
(d)在一个独立的压力容器中同时注入硫酸、加热的蒸馏水和硫酸铵(混合物I)结合；
(e)加热压力混合物至约200-1200约30分钟形成混合物(II)；
(f)冷却混合物(II)并向该冷却的混合物中加入混合物(I)的稳定剂部分，该稳定剂是混合物(I)占混合物(II)总重量的约10％重量；
(g)加入含有金属离子的化合物以形成稳定的悬浮液(混合物III)；
(h)稀释金属离子悬浮液以形成有效的抗微生物组合物；和
(I)向食物和非食物施应用该抗微生物组合物。
22.权利要求21的方法，其中所述的金属离子选自由铜离子、银离子、锌离子、镁离子及其混合物组成的组。
23.权利要求21的方法，其中所述的含有金属离子的化合物至少选自以下一种：硫酸铜、五水硫酸铜、谷氨酸铜、氧化锌、谷氨酸锌、谷氨酸镁、硫酸镁、氧化银和硫酸银组成的组。
24.一种稳定的抗微生物混合物，包括金属离子、硫酸、硫酸铵和蒸馏水，其中金属离子在pH值范围为约0-9、温度约为32-212的范围内保持悬浮。
25.权利要求24的抗微生物混合物，其中所述的金属盐至少选自以下一种化合物：硫酸铜、五水硫酸铜、谷氨酸铜、氧化锌、谷氨酸锌、谷氨酸镁、硫酸镁、氧化银和硫酸银。
26.权利要求25的抗微生物混合物，其中所述的金属盐含有的离子选自由铜离子、银离子、锌离子、镁离子及其混合物组成的组。
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| EP1722638A4 (en) | 2009-08-26 |
| US20050191395A1 (en) | 2005-09-01 |
| WO2005082069A2 (en) | 2005-09-09 |
| WO2005082069A3 (en) | 2006-10-05 |
| MXPA06009797A (es) | 2007-08-14 |
| CN101076256A (zh) | 2007-11-21 |
| EP1791578A2 (en) | 2007-06-06 |
| CA2599345A1 (en) | 2005-10-06 |
| US20050191394A1 (en) | 2005-09-01 |
| WO2005082071A2 (en) | 2005-09-09 |
| WO2005091739A2 (en) | 2005-10-06 |
| EP1729581A2 (en) | 2006-12-13 |
| MXPA06009800A (es) | 2007-04-24 |
| WO2005091739A3 (en) | 2007-05-24 |
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