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CN100396641C - 磷酸镁铵水泥制剂,生产方法和用途与生产该水泥的方法 - Google Patents

磷酸镁铵水泥制剂,生产方法和用途与生产该水泥的方法 Download PDF

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CN100396641C
CN100396641C CNB018018157A CN01801815A CN100396641C CN 100396641 C CN100396641 C CN 100396641C CN B018018157 A CNB018018157 A CN B018018157A CN 01801815 A CN01801815 A CN 01801815A CN 100396641 C CN100396641 C CN 100396641C
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aqueous solution
powdered mixture
ammonium
cement
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CN1383420A (zh
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M·奇莫曼
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Sanatis GmbH
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Abstract

本发明涉及水泥，硬化后其主相由磷酸镁铵微晶和纳米磷灰石组成，并同时具有高强度。该材料是生物可降解的并适用于牙齿水泥，作为骨代用品，骨填料，骨水泥或骨粘附材料。

Description

磷酸镁铵水泥制剂，生产方法和用途与生产该水泥的方法
技术领域
本发明涉及磷酸镁铵水泥制剂，其生产方法和有关的用途。
本发明尤其涉及生物可降解的水泥，所述水泥硬化后其主相由磷酸镁铵和纳米磷灰石组成并同时具有高强度。该材料可用作骨代用品，用于骨增强和骨再生。它也可用作药物或生物活性物质的载体材料。
背景技术
构成人骨和牙釉组织的最重要的矿物组成是钙和磷酸盐。但是，也存在大量的钠、镁和碳酸盐。由合成系统的沉淀研究已知：钠离子和碳酸盐离子极易掺入磷酸钙沉淀物中，形成与磷灰石类似的分子结构。当然，镁也极容易沉积，其结构与磷灰石的结构不同。
生理上用作骨和牙质的沉淀磷酸钙是纳米晶体。从X射线衍射图上不能区分它们是磷灰石，还是其他结构，这是因为衍射线变宽的缘故。有一些科学家持这样的观点：在骨和牙质中存在大量的镁，以致于它们不能全部进入磷灰石结构中。因此，在这里假定是由纳米磷灰石和纳米白云石或纳米鸟粪石构成的矿物的混合形式。磷酸钙不仅是生物相容的，而且作为人体属性的生存细胞被识别。因此，有许多生物材料和部分由磷酸钙构成的医学产品。
大约自1970年以来，市场上出现了部分以预制块或颗粒形式存在的磷酸钙陶瓷。这些材料在骨结构中的植入取得了很大的成功。该体系最大的不足是块体需要预制并且颗粒从植入侧滑移掉(冲掉)。这常常导致这类的植入失败。
由羟基磷灰石(HA)或β-磷酸三钙(β-TCP，白磷钙石状结构)或者由这两者，HA和β-TCP以可变比例构成的磷酸钙陶瓷是最成功的。HA实际上不再由骨植入体吸收，而β-TCP则缓慢地被吸收并被新骨置换。因此，改变β-TCP/HA的比例会影响磷酸钙陶瓷的吸收程度。同样可混合其他的再吸收材料，例如三斜磷钙石CaHPO4、透钙磷石CaHPO4-2H2O、方解石CaCO3和白云石CaMg(CO3)2。
自1985年以来，人们试图开发磷酸钙水泥，以便克服预制或颗粒状磷酸钙陶瓷存在的缺点(W.E.Brown和L.C.Chow，“A new calcium phosphate，water-setting cement”，Cem.Res.Prog.1986 352-379(1987))。这包括尚未进入商业化的透钙磷石水泥，沉淀相的Ca/P摩尔比为1.00。该相不是纳米晶体，而是微米晶体。迄今为止开发的所有其他磷酸钙水泥具有纳米晶体的沉淀结构并且Ca/P摩尔比≥1.5，通过添加碳酸盐可进一步提高该摩尔比。美国专利US5605713；欧洲专利申请EP0835668A1；WO96/14265公开了这些材料；市场上已经有一些这类材料。有关这些材料在植入骨和软组织后的再吸收性出现了相互矛盾的报道。在每一种情况下，不再可吸收的羟基磷灰石(HA)(参见上述的HA陶瓷)基磷酸钙水泥与骨转导性良好的缺钙羟基磷灰石(CDHA，缺钙的羟基磷灰石)基磷酸钙水泥不同。最后提及的情况是指：它们可被破骨细胞再吸收并且可被来自破骨细胞的新骨组织置换掉。这些水泥的再吸收主要是取决于局部的骨转换机理。今天，大多数的外科医生需要的是磷酸钙水泥，其中首先是机械支承的有效方式发挥了作用，但是，最后的再吸收与骨的局部转换机理无关，即材料完全地降解掉。另外，在外科矫正畸形术中，已知活骨仅仅维持在从生物力学的观点出发所需的位置上。这作为所谓的Wolff′s定律是已知的。因此，如果补入骨缺损处的磷酸钙水泥，具有的抗压强度要比其周围的骨高，并且该高抗压强度保持不变，则导致植入体(这里是磷酸钙水泥)周围的骨组织降解。
为了满足这种需要，即便是仅仅满足部分需要，某些制造商已经将这些物质混入与纳米磷灰石类似的CDHA水泥中，这种水泥因浓度梯度被动地被体液再吸收，例如三斜磷钙石(CaHPO4)或方解石(CaCO3)，如欧洲专利EP0543765公开的。
但是，这仅仅是部分地解决了问题。还需要一种能够完全被动地再吸收的水泥，其中再吸收端和沉积端直接进行接触。例如，石膏不能满足这种要求。石膏快速地被再吸收，以致于在再吸收端和沉积端之间总是有空穴存在，这些材料因其抗压强度低不能起充分支承的作用。例如，美国专利US5281265公开了这类材料。
基于该原因，需要提供一种骨替代材料，首先起具有高抗压强度的骨所失去的支承作用，然后逐步地降低抗压强度，结果刺激内源骨的转换过程(重新生长)，因此，快速地进行骨再生(osteoneogenesis)并因此使骨替代材料进行有效的再吸收。这还可通过加入微溶性的物质实现，例如，将它们加入硬化的水泥浆料中。因为骨很好地生长成微孔结构，因此，有利的是将由诸如糖、盐(例如NaCl)或石膏(CaSO4)组成的颗粒或丸粒状可溶性物质混合到水泥浆料中。然后它们从硬化的水泥结构中浸出，快速地进入体内，并保持多孔的海绵状结构。在体外侧生产多孔(制好的)水泥也是可能的。
为了能使水泥用于牙科领域，例如填补和密封小的牙槽，填补活牙摘除后的牙洞，采用这样的一种水泥作为牙髓病学中的辅助填补材料，这样的一种材料不会收缩，防止了细菌的通过。甚至对具有较低可膨胀特性的材料也有需求。
发明内容
本发明的目的是提供一种水泥制剂，利用该水泥制剂克服了现有技术的缺陷。
因此，本发明提供了一种磷酸镁铵水泥制剂，含有
-粉末混合物，混合物中含有正磷酸钙和正磷酸镁，其中钙与正磷酸根的摩尔比是大于1.00和小于1.50，和其中镁与正磷酸根的摩尔比是大于0和小于0.50，
-一种铵盐；和
-水和/或水溶液。
在一个实施方案中，优选地水溶液是pH值在7＜pH＜12范围内的铵盐水溶液。
进一步优选地，铵盐是存在于粉末混合物中的，各组分钙(Ca)、镁(Mg)、正磷酸根(P)和铵(NH4)的摩尔量在1.00＜Ca/P＜1.50和0＜Mg/P＜0.50和0＜NH4＜0.50的范围内。
更进一步地，粉末混合物含有α/β-磷酸三钙(α/β-TCP)和优选MgHPO4×3H2O。
此外，粉末混合物除了α/β-TCP和MgHPO4×3H2O外，另外含有Mg3(PO4)2。
在本发明的一个方面，水溶液包括(NH4)2SO4水溶液。
在另一个方面，粉末混合物含有(NH4)2SO4。
优选地，水溶液由(NH4)2HPO4水溶液组成。
此外，粉末混合物还含有KH2PO4，或者粉末混合物还含有Na2HPO4，和/或所述制剂还含有SrCO3。优选地，SrCO3的含量按制剂的总量计为0.01-10％(重量)，优选0.1-5％(重量)。
根据本发明，还提供了一种磷酸镁铵水泥制剂，含有
-一种由α-TCP，β-TCP，MgHPO4×3H2O，KH2PO4和Na2HPO4组成的粉末混合物；
-一种铵盐；和
水和/或一种水溶液。
根据本发明的进一步构成，还提供了一种磷酸镁铵水泥制剂，含有
-一种由α/β-TCP，MgHPO4×3H2O，KH2PO4，Na2HPO4和Mg3(PO4)2和一种含铵离子的水溶液组成的粉末混合物。
优选地，在上述的制剂中含有铵盐的水溶液作为水溶液。
根据再一方面，提供了一种磷酸镁铵水泥制剂，含有
-一种由α-TCP，β-TCP，(NH4)2SO4，KH2PO4和Na2HPO4组成的粉末混合物；
-一种镁盐，优选MgHPO4×3H2O；和
-水和/或一种水溶液。
同样地，该制剂优选含有镁盐的水溶液作为水溶液。
根据进一步方面，本发明提供再一个磷酸镁铵水泥制剂，含有
-一种由α-TCP，β-TCP，伯或仲磷酸铵，KH2PO4和Na2HPO4组成的粉末混合物；
-一种镁盐，优选MgHPO4×3H2O；和
-水和/或一种水溶液。
根据本发明的上述制剂在粉末混合物中还含有SrCO3，其含量按制剂的总量计优选占0.01-10％(重量)。
这些制剂优选含有锶盐的水溶液作为水溶液。
进一步地，粉末混合物和/或水溶液中含有作为附加组分的ZnO。此外，粉末混合物还含有Ca2NaK(PO4)2和/或CaKPO4。
在一个进一步方案中，粉末混合物和/或水溶液中含有作为附加组分的氟离子。
进一步地，粉末混合物和/或混合液体中含有作为附加组分的药物和/或生物活性组分，优选治疗剂量的抗生素、细胞生长抑制剂、止痛药、消毒剂、生长因子、蛋白质或弹性蛋白抑制剂。
本发明也提供了上述磷酸镁铵水泥制剂的生产方法，其中使粉末混合物与混合液体混合，同时使液体均匀地分布在粉末混合物中，将由此获得的浆料施加在目标区域上或施加到目标区域中或输送到目标区域中并使其硬化，其中各组分发生反应，致使形成的水泥具有磷酸镁铵微晶。
根据另一方面，本发明提供了这样的一种采用所述磷酸镁铵制剂生产磷酸镁铵水泥的方法，其中使粉末混合物与混合液体混合，同时使溶液均匀地分布在粉末混合物中，将由此获得的浆料施加在目标区域上或施加到目标区域中，或输送到目标区域中，并使得到的水泥硬化，形成磷酸镁铵微晶。
在这样的方法中，优选地将粒状的，易溶于含水液体中的颗粒添加到粉末混合物中，粒径为约10-300微米，优选50-200微米。
其中粒状颗粒优选由NaCl，糖，CaSO4，β-TCP，聚丙交酯、聚乙交酯或聚丙交酯/聚乙交酯共聚物，CaCO3和CaHPO4组成。
本发明还提供了上述制剂的用途，用于医学目的，例如用作牙齿水泥，或用作骨代用品或骨填料或骨水泥或骨粘附材料。
具体实施方式
现有技术存在的问题优选按照本发明有效地解决，其中通过改变锶盐的混合调节硬化水泥浆料的膨胀能力。在试验中，如实施例所示的，即示出了水泥混合物的膨胀能力，其主相在硬化状态下是磷酸镁铵，随着总粉末混合物中的锶盐的重量比增加而降低。因此，借助本发明，可以提供用于牙髓病学的材料，这种材料除了具有足够的抗机械稳定性外，还具有可膨胀性。
-本发明的目的是提供一种骨代用品、骨增强和骨再生用的材料，这种材料在有限的时间内可被吸收并且其抗压性降低到与体再生的要求相适应。
-同样，本发明的目的是提供一种在标准温度条件下，优选在体温下可生产、制备和模制的材料，即水泥。
所提供材料的特征是可通过其加工时间内，尤其是在室温下引入的Mg3(PO4)2的烧结程度的强度额外地进行调节，其中在这些颗粒的表面上的溶解速率受烧结的程度和由此形成的所使用的Mg3(PO4)2的密度控制，以便可以控制固化所需的沉积Ca/Mg/磷酸盐化合物的沉淀。
-此外，本发明的目的是提供一种具有部分溶解性的磷酸盐水泥，优选是因磷酸镁铵磷灰石结构(水泥)的缓慢溶解引起的。
-此外，本发明的目的是提供一种反应方法，该方法导致从数个单独的组分形成磷酸镁铵水泥，并在临床可接受的时间内在室温和/或体温下硬化。
-此外，本发明的目的是提供一种在临床可接受的时间内变成足够硬化和稳定的并对矿质表面具有强粘附能力的材料。
-此外，本发明的目的是提供本发明公开的材料，其特征在于对金属表面具有强粘附能力。
-此外，本发明的目的是提供一种可再吸收的水泥，这种水泥能以混合浆料的形式注入。
-本发明的一个方面是最终产品由粉末混合物组成，具有的Ca/P摩尔比在1.00-1.50的范围内(P代表正磷酸盐)。
-另外，该粉末混合物的Mg/P的摩尔比在0-1.00的范围内是重要的。
-为了混合和形成在可接受时间内硬化的水泥浆料，这些粉末混合物必需具有足够活性。为了实现这一目的，本发明的其他方面是用适量的稍呈碱性(7＜pH＜12)的可溶离子组分的水溶液，例如Na3PO4、K2CO3和/或Na2CO3与(NH4)2HPO4的混合水溶液混合粉末混合物。
-本发明的其他特征是将粒状的但在体液中易溶的粒状固体混合到硬化水泥浆料中，以便在其溶出后形成微孔至大孔的体系。
-本发明的其他方面是在几小时内使这些水泥达到其最大强度。
-本发明的其他特征是在凝固期间水泥的膨胀能力。膨胀性是通过混合的锶盐的相对比例确定或调节的。
-本发明的其他特征是硬化的水泥由微晶磷酸镁铵组成。
-本发明的其他特征水泥的起始硬化时间可设定在1-40分钟，最终硬化时间设定在2.5-60分钟(根据ASTM C266-89)。
-本发明的其他特征是水泥的抗压强度最大可达到50Mpa以上。
-本发明的其他特征是在达到初始硬化时间前水泥浆料可注射。
-本发明的其他特征是水泥浆料可起其他材料(不是Ca、Mg和/或磷酸盐的材料)的载体的作用。例如ZnO、药物活性组分(抗生素、细胞生长抑制剂、生长因子)或其他生物活性物质。
由实施例的描述可以看出本发明的其他特征和优点。
实施例：
在实施例中使用了下列符号：
PM＝粉末混合物
L＝液体
L/PM＝液体/粉末比，按ml/g计
ti＝初始硬化时间(按照ASTM标准C266-89，Gilmoore needle)
tF＝最终硬化时间(按照ASTM标准C266-89，Gilmoore needle)
D(x h)＝在37℃下，储存在0.9％强NaCl溶液中x小时后的抗压强度，按Mpa计。
生产：在称重所有的组分后，用球磨机均化混合粉末混合物约20分钟。
实施例1：
Figure C0180181500161
实施例2：
Figure C0180181500171
实施例3：
Figure C0180181500172
实施例4：
实施例5：
Figure C0180181500181
实施例6：
Figure C0180181500182
实施例7：
Figure C0180181500183
实施例8：
实施例9：
Figure C0180181500192
实施例10：
Figure C0180181500201
实施例11：
Figure C0180181500202
实施例12：
Figure C0180181500211
实施例13：
Figure C0180181500212
实施例14：
Figure C0180181500221
实施例15：
Figure C0180181500222
实施例16：
实施例17：
PM＝60g α-TCP+6g Mg3(PO4)2+10g KH2PO4+5g β-TCP
混合溶液：3.2摩尔浓度溶液(NH4)2HPO4
L/PM＝0,35
Ti＝10,8  tf＝20
D(2)＝18,5±1,0
D(18)＝48,3±1,8

Claims (111)

1.磷酸镁铵水泥制剂，含有
-粉末混合物，混合物中含有正磷酸钙和正磷酸镁，其中钙与正磷酸根的摩尔比是大于1.00和小于1.50，和其中镁与正磷酸根的摩尔比是大于0和小于0.50，
-一种铵盐；和
-水和/或水溶液。
2.根据权利要求1的制剂，其中水溶液是pH值在7＜pH＜12范围内的铵盐水溶液。
3.根据权利要求1的制剂，其中铵盐是存在于粉末混合物中的，其中铵的摩尔量在大于0和小于0.50的范围内。
4.根据权利要求1-3任一项的制剂，其中粉末混合物含有α/β-磷酸三钙。
5.根据权利要求1-3任一项的制剂，其中粉末混合物含有MgHPO4×3H2O。
6.根据权利要求1-3任一项的制剂，其中粉末混合物除了α/β-磷酸三钙和MgHPO4×3H2O外，另外含有Mg3(PO4)2。
7.根据权利要求1-3任一项的制剂，其中水溶液包括(NH4)2SO4水溶液。
8.根据权利要求1-3任一项的制剂，其中粉末混合物含有(NH4)2SO4。
9.根据权利要求1-3任一项的制剂，其中水溶液由(NH4)2HPO4水溶液组成。
10.根据权利要求1-3任一项的制剂，其中粉末混合物还含有KH2PO4。
11.根据权利要求1-3任一项的制剂，其中粉末混合物还含有Na2HPO4。
12.根据权利要求1-3任一项的制剂，还含有SrCO3。
13.根据权利要求12的制剂，其中SrCO3的含量按制剂的总量计为0.01-10％重量。
14.根据权利要求13的制剂，其中SrCO3的含量按制剂的总量计为0.1-5％重量。
15.根据权利要求1-3任一项的制剂，含有锶盐的水溶液作为水溶液。
16.根据权利要求1-3任一项的制剂，粉末混合物和/或水溶液中含有作为附加组分的ZnO。
17.根据权利要求1-3任一项的制剂，其中粉末混合物还含有Ca2NaK(PO4)2和/或CaKPO4。
18.根据权利要求1-3任一项的制剂，粉末混合物和/或水溶液中含有作为附加组分的氟离子。
19.根据权利要求1-3任一项的制剂，粉末混合物和/或水溶液中含有作为附加组分的药物和/或生物活性组分。
20.根据权利要求19的制剂，粉末混合物和/或水溶液中含有治疗剂量的抗生素、细胞生长抑制剂、止痛药、消毒剂、生长因子、蛋白质或弹性蛋白抑制剂。
21.权利要求1-20任一项的磷酸镁铵水泥制剂的生产方法，其中使粉末混合物与水溶液混合，同时使液体均匀地分布在粉末混合物中。
22.根据权利要求21的方法，其中该方法产生易溶于含水液体中的颗粒，粒径为10-300微米。
23.根据权利要求22的方法，其中所述粒径为50-200微米。
24.根据权利要求22的方法，其中粒状颗粒由NaCl，糖，CaSO4，β-磷酸三钙，聚丙交酯、聚乙交酯或聚丙交酯/聚乙交酯共聚物，CaCO3和CaHPO4组成。
25.采用权利要求1-20任一项的磷酸镁铵制剂生产磷酸镁铵水泥的方法，其中使粉末混合物与水溶液混合，同时使溶液均匀地分布在粉末混合物中，将由此获得的浆料施加在目标区域上或施加到目标区域中，或输送到目标区域中，并使得到的水泥硬化，形成磷酸镁铵微晶。
26.根据权利要求25的方法，其中该方法产生易溶于含水液体中的颗粒添，粒径为10-300微米。
27.根据权利要求26的方法，其中所述粒径为50-200微米。
28.根据权利要求26的方法，其中粒状颗粒由NaCl，糖，CaSO4，β-磷酸三钙，聚丙交酯、聚乙交酯或聚丙交酯/聚乙交酯共聚物，CaCO3和CaHPO4组成。
29.根据权利要求1-20任一项的制剂的用途，用作牙齿水泥。
30.根据权利要求1-20任一项的制剂的用途，用作骨代用品或骨填料或骨水泥或骨粘附材料。
31.磷酸镁铵水泥制剂，含有
-一种由α-磷酸三钙，β-磷酸三钙，MgHPO4×3H2O，KH2PO4和Na2HPO4组成的粉末混合物；
-一种铵盐；和
-水和/或一种水溶液。
32.根据权利要求31的制剂，含有铵盐的水溶液作为水溶液。
33.根据权利要求31或32的制剂，粉末混合物中还含有SrCO3。
34.根据权利要求33的制剂，其中SrCO3的含量按制剂的总量计占0.01-10％重量。
35.根据权利要求31或32的制剂，含有锶盐的水溶液作为水溶液。
36.根据权利要求31或32的制剂，粉末混合物和/或水溶液中含有作为附加组分的ZnO。
37.根据权利要求31或32的制剂，其中粉末混合物还含有Ca2NaK(PO4)2和/或CaKPO4。
38.根据权利要求31或32的制剂，粉末混合物和/或水溶液中含有作为附加组分的氟离子。
39.根据权利要求31或32的制剂，粉末混合物和/或水溶液中含有作为附加组分的药物和/或生物活性组分。
40.根据权利要求39的制剂，其中粉末混合物和/或水溶液中含有治疗剂量的抗生素、细胞生长抑制剂、止痛药、消毒剂、生长因子、蛋白质或弹性蛋白抑制剂。
41.权利要求31-40任一项的磷酸镁铵水泥制剂的生产方法，其中使粉末混合物与水溶液混合，同时使液体均匀地分布在粉末混合物中。
42.根据权利要求41的方法，其中该方法产生易溶于含水液体中的颗粒，粒径为10-300微米。
43.根据权利要求42的方法，其中所述粒径为50-200微米。
44.根据权利要求42的方法，其中粒状颗粒由NaCl，糖，CaSO4，β-磷酸三钙，聚丙交酯、聚乙交酯或聚丙交酯/聚乙交酯共聚物，CaCO3和CaHPO4组成。
45.采用权利要求31-40任一项的磷酸镁铵制剂生产磷酸镁铵水泥的方法，其中使粉末混合物与水溶液混合，同时使溶液均匀地分布在粉末混合物中，将由此获得的浆料施加在目标区域上或施加到目标区域中，或输送到目标区域中，并使得到的水泥硬化，形成磷酸镁铵微晶。
46.根据权利要求45的方法，其中该方法产生易溶于含水液体中的颗粒，粒径为10-300微米。
47.根据权利要求46的方法，其中所述粒径为50-200微米。
48.根据权利要求46的方法，其中粒状颗粒由NaCl，糖，CaSO4，β-磷酸三钙，聚丙交酯、聚乙交酯或聚丙交酯/聚乙交酯共聚物，CaCO3和CaHPO4组成。
49.根据权利要求31-40任一项的制剂的用途，用作牙齿水泥。
50.根据权利要求31-40任一项的制剂的用途，用作骨代用品或骨填料或骨水泥或骨粘附材料。
51.磷酸镁铵水泥制剂，含有
-一种由α/β-磷酸三钙，MgHPO4×3H2O，KH2PO4，Na2HPO4和Mg3(PO4)2组成的粉末混合物和一种含铵离子的水溶液。
52.根据权利要求51的制剂，含有铵盐的水溶液作为水溶液。
53.根据权利要求51或52的制剂，粉末混合物中还含有SrCO3。
54.根据权利要求53的制剂，其中SrCO3的含量按制剂的总量计占0.01-10％重量。
55.根据权利要求51或52的制剂，含有锶盐的水溶液作为水溶液。
56.根据权利要求51或52的制剂，粉末混合物和/或水溶液中含有作为附加组分的ZnO。
57.根据权利要求51或52的制剂，其中粉末混合物还含有Ca2NaK(PO4)2和/或CaKPO4。
58.根据权利要求51或52的制剂，粉末混合物和/或水溶液中含有作为附加组分的氟离子。
59.根据权利要求51或52的制剂，粉末混合物和/或水溶液中含有作为附加组分的药物和/或生物活性组分。
60.根据权利要求59的制剂，其中粉末混合物和/或水溶液中含有治疗剂量的抗生素、细胞生长抑制剂、止痛药、消毒剂、生长因子、蛋白质或弹性蛋白抑制剂。
61.权利要求51-60任一项的磷酸镁铵水泥制剂的生产方法，其中使粉末混合物与水溶液混合，同时使液体均匀地分布在粉末混合物中。
62.根据权利要求61的方法，其中该方法产生易溶于含水液体中的颗粒，粒径为10-300微米。
63.根据权利要求62的方法，其中所述粒径为50-200微米。
64.根据权利要求62的方法，其中粒状颗粒由NaCl，糖，CaSO4，β-磷酸三钙，聚丙交酯、聚乙交酯或聚丙交酯/聚乙交酯共聚物，CaCO3和CaHPO4组成。
65.采用权利要求51-60任一项的磷酸镁铵制剂生产磷酸镁铵水泥的方法，其中使粉末混合物与水溶液混合，同时使溶液均匀地分布在粉末混合物中，将由此获得的浆料施加在目标区域上或施加到目标区域中，或输送到目标区域中，并使得到的水泥硬化，形成磷酸镁铵微晶。
66.根据权利要求65的方法，其中该方法产生易溶于含水液体中的颗粒，粒径为10-300微米。
67.根据权利要求66的方法，其中所述粒径为50-200微米。
68.根据权利要求66的方法，其中粒状颗粒由NaCl，糖，CaS4，β-磷酸三钙，聚丙交酯、聚乙交酯或聚丙交酯/聚乙交酯共聚物，CaCO3和CaHPO4组成。
69.根据权利要求51-60任一项的制剂的用途，用作牙齿水泥。
70.根据权利要求51-60任一项的制剂的用途，用作骨代用品或骨填料或骨水泥或骨粘附材料。
71.磷酸镁铵水泥制剂，含有
-一种由α-磷酸三钙，β-磷酸三钙，(NH4)2SO4，KH2PO4和Na2HPO4组成的粉末混合物；
-一种镁盐，和
-水和/或一种水溶液。
72.根据权利要求71的制剂，其中所述镁盐是MgHPO4×3H2O。
73.根据权利要求71或72的制剂，含有镁盐的水溶液作为水溶液。
74.根据权利要求71或72的制剂，粉末混合物中还含有SrCO3。
75.根据权利要求74的制剂，其中SrCO3的含量按制剂的总量计占0.01-10％重量。
76.根据权利要求71或72的制剂，含有锶盐的水溶液作为水溶液。
77.根据权利要求71或72的制剂，粉末混合物和/或水溶液中含有作为附加组分的ZnO。
78.根据权利要求71或72的制剂，其中粉末混合物还含有Ca2NaK(PO4)2和/或CaKPO4。
79.根据权利要求71或72的制剂，粉末混合物和/或水溶液中含有作为附加组分的氟离子。
80.根据权利要求71或72的制剂，粉末混合物和/或水溶液中含有作为附加组分的药物和/或生物活性组分。
81.根据权利要求80的制剂，其中粉末混合物和/或水溶液含有治疗剂量的抗生素、细胞生长抑制剂、止痛药、消毒剂、生长因子、蛋白质或弹性蛋白抑制剂。
82.权利要求71-81任一项的磷酸镁铵水泥制剂的生产方法，其中使粉末混合物与水溶液混合，同时使液体均匀地分布在粉末混合物中。
83.根据权利要求82的方法，其中该方法产生易溶于含水液体中的颗粒，粒径为10-300微米。
84.根据权利要求83的方法，其中所述粒径为50-200微米。
85.根据权利要求83的方法，其中粒状颗粒由NaCl，糖，CaSO4，β-磷酸三钙，聚丙交酯、聚乙交酯或聚丙交酯/聚乙交酯共聚物，CaCO3和CaHPO4组成。
86.采用权利要求71-81任-项的磷酸镁铵制剂生产磷酸镁铵水泥的方法，其中使粉末混合物与水溶液混合，同时使溶液均匀地分布在粉末混合物中，将由此获得的浆料施加在目标区域上或施加到目标区域中，或输送到目标区域中，并使得到的水泥硬化，形成磷酸镁铵微晶。
87.根据权利要求86的方法，其中该方法产生易溶于含水液体中的颗粒，粒径为10-300微米。
88.根据权利要求87的方法，其中所述粒径为50-200微米。
89.根据权利要求87的方法，其中粒状颗粒由NaCl，糖，CaSO4，β-磷酸三钙，聚丙交酯、聚乙交酯或聚丙交酯/聚乙交酯共聚物，CaCO3和CaHPO4组成。
90.根据权利要求71-81任一项的制剂的用途，用作牙齿水泥。
91.根据权利要求71-81任一项的制剂的用途，用作骨代用品或骨填料或骨水泥或骨粘附材料。
92.磷酸镁铵水泥制剂，含有
-一种由α-磷酸三钙，β-磷酸三钙，伯或仲磷酸铵，KH2PO4和Na2HPO4组成的粉末混合物；
-一种镁盐，
-水和/或水溶液。
93.根据权利要求92的制剂，其中所述镁盐是MgHPO4×3H2O。
94.根据权利要求92或93的制剂，粉末混合物中还含有SrCO3。
95.根据权利要求94的制剂，其中SrCO3的含量按制剂的总量计占0.01-10％重量。
96.根据据权利要求92或93的制剂，含有锶盐的水溶液作为水溶液。
97.根据权利要求92或93的制剂，粉末混合物和/或水溶液中含有作为附加组分的ZnO。
98.根据权利要求92或93的制剂，其中粉末混合物还含有Ca2NaK(PO4)2和/或CaKPO4。
99.根据权利要求92或93的制剂，粉末混合物和/或水溶液中含有作为附加组分的氟离子。
100.根据权利要求92或93的制剂，粉末混合物和/或水溶液中含有作为附加组分的药物和/或生物活性组分。
101.根据权利要求100的制剂，其中粉末混合物和/或水溶液中含有治疗剂量的抗生素、细胞生长抑制剂、止痛药、消毒剂、生长因子、蛋白质或弹性蛋白抑制剂。
102.权利要求92-101任一项的磷酸镁铵水泥制剂的生产方法，其中使粉末混合物与水溶液混合，同时使液体均匀地分布在粉末混合物中。
103.根据权利要求102的方法，其中该方法产生易溶于含水液体中的颗粒，粒径为10-300微米。
104.根据权利要求103的方法，其中所述粒径为50-200微米。
105.根据权利要求103的方法，其中粒状颗粒由NaCl，糖，CaSO4，β-磷酸三钙，聚丙交酯、聚乙交酯或聚丙交酯/聚乙交酯共聚物，CaCO3和CaHPO4组成。
106.采用权利要求92-101任一项的磷酸镁铵制剂生产磷酸镁铵水泥的方法，其中使粉末混合物与水溶液混合，同时使溶液均匀地分布在粉末混合物中，将由此获得的浆料施加在目标区域上或施加到目标区域中，或输送到目标区域中，并使得到的水泥硬化，形成磷酸镁铵微晶。
107.根据权利要求106的方法，其中该方法产生易溶于含水液体中的颗粒，粒径为10-300微米。
108.根据权利要求107的方法，其中所述粒径为50-200微米。
109.根据权利要求107的方法，其中粒状颗粒由NaCl，糖，CaSO4，β-磷酸三钙，聚丙交酯、聚乙交酯或聚丙交酯/聚乙交酯共聚物，CaCO3和CaHPO4组成。
110.根据权利要求92-101任一项的制剂的用途，用作牙齿水泥。
111.根据权利要求92-101任一项的制剂的用途，用作骨代用品或骨填料或骨水泥或骨粘附材料。
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US20090221717A1 (en) 2009-09-03
US7431763B2 (en) 2008-10-07
US20040173122A1 (en) 2004-09-09
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US20050246036A1 (en) 2005-11-03
AU2001279710A1 (en) 2002-01-14
US20020166480A1 (en) 2002-11-14
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US20080020980A1 (en) 2008-01-24
US20100173846A1 (en) 2010-07-08
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US20070022912A1 (en) 2007-02-01
DE10032220A1 (de) 2002-01-24
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US6908506B2 (en) 2005-06-21
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US7540914B2 (en) 2009-06-02
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