CN106008769B - 用于放射治疗三维剂量验证的凝胶的制备方法及应用 - Google Patents
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Abstract
本发明涉及一种用于放射治疗三维剂量验证的凝胶的制备方法，包括以下步骤：将油溶性聚合单体与水混合，得到第一溶液；将第一溶液除氧，然后放入γ射线源，辐照交联，得到溶解了聚合物的第二溶液，离心，冷冻干燥，得到聚合物微球固体粉末；将聚合物微球固体粉末与辐射发光单体在水中混合，得到第三溶液，将水溶性聚合单体溶于水中，得到第四溶液；将第三溶液和第四溶液混合，除氧，然后放入γ射线源，辐照交联，得到用于放射治疗三维剂量验证的凝胶。该制备方法快速简单、成本低廉、产量大、无其他副产物，合成的凝胶具有良好的发光效率、良好的机械强度，且具有很好的组织等效性，便于本发明中的凝胶剂量计在临床放疗过程中的剂量验证。
Description
技术领域
本发明涉及放射治疗剂量验证领域，尤其涉及一种用于放射治疗三维剂量验证的凝胶的制备方法及应用。
背景技术
现阶段，癌症治疗的主要方式有手术治疗，化学治疗和放射治疗。据2014年WHO组织统计显示，70％以上的癌症患者需要采用单独放疗或与放疗结合的手段进行治疗。
放射治疗作为一种重要的手段，在癌症治疗中发挥着越来越重要的作用。但放射治疗癌症的最大缺陷是无选择性的破坏，即在射线能量沉积的区域，在杀死肿瘤细胞的同时，也会对人体正常细胞造成伤害。因此整个放射治疗过程中，设定精准的放射治疗计划以控制剂量的分布和降低正常细胞的并发症显得尤为重要。因此，精准的治疗计划和剂量验证技术将有效提高放疗效果，减少副作用的产生，其发展具有必要性和迫切性。
然而目前剂量验证技术并没有突破性的发展，现阶段放射治疗过程中的剂量验证仍然主要以一维点剂量或二维面剂量来验证整个放射治疗过程中三维(3D)剂量的沉积分布，再结合计算机模拟技术制定放疗方案。点面剂量验证技术已不能完全满足现代放疗对于三维吸收剂量与剂量梯度测量准确性和精准性的要求。因此精准的剂量验证技术是高精确放射治疗技术可靠用于临床并保证治疗质量的前提，精准、快速、个性化将是放疗剂量验证技术未来的发展趋势。而三维水凝胶剂量计能真实地反映放射治疗中靶区组织受辐射的三维剂量分布情况，因此可以满足放射治疗技术发展的要求，是当今国际放疗领域的一项重大课题，也是未来剂量验证的主要发展方向。凝胶剂量材料是三维凝胶剂量计的核心组成部分，决定了放疗剂量验证的精确性和准确性。因此研制可重复利用、机械强度良好、响应灵敏、组织等效性优异的剂量验证材料具有非常重要的实际应用价值。
目前放射治疗过程中广泛使用的3D剂量验证技术是利用三维水箱模拟生物组织的辐射吸收和散射状态，再结合剂量探测器进行3D剂量分布的验证。三维水箱可以比较准确的测量单束射线固定照射过程中剂量的分布，但并不能满足复杂照射条件(动态照射条件、复杂照射野等)下的剂量验证。此外人体体模也用于剂量验证，但受制于探测器数量和体模昂贵的价格，并不适应于放疗过程中常规的剂量验证。
高分子因其组织等效性和成分近似性而被应用于剂量验证，其中水凝胶材料是研究最多的一类高分子材料。
鉴于上述缺陷，本设计人积极加以研究创新，以期创设一种用于放射治疗三维剂量验证的凝胶材料的制备方法及应用，使其更具有产业上的利用价值。
发明内容
为解决上述技术问题，本发明的目的是提供一种用于放射治疗三维剂量验证的凝胶材料的制备方法及应用，该制备方法快速简单，且成本低廉、产量大、无其他副产物，合成的材料具有良好的发光效率，同时提高了材料的强度，且具有很好的组织等效性，便于本发明中的凝胶剂量计在临床放疗过程中的剂量验证。
本发明的一种用于放射治疗三维剂量验证的凝胶的制备方法，包括以下步骤：
(1)将油溶性聚合单体与水混合，得到第一溶液；
(2)将步骤(1)中的第一溶液除氧，然后放入γ射线源中辐照交联，得到含有聚合物的第二溶液，离心，冷冻干燥，得到聚合物微球固体粉末；
(3)将步骤(2)得到的聚合物微球固体粉末与辐射发光单体在水中混合，得到第三溶液，将水溶性聚合单体溶于水中，得到第四溶液；
(4)将步骤(3)中的第三溶液和第四溶液混合，除氧，然后放入γ射线源中辐照交联，得到用于放射治疗三维剂量验证的凝胶。
进一步的，在步骤(1)中，油溶性聚合单体为苯乙烯(St)、4-苯基-1-丁烯、烯丙苯、对甲基苯乙烯、间甲基苯乙烯、丙烯酸甲酯，丙烯酸丁酯和丙烯酸丙酯中的一种或几种。
进一步的，在步骤(1)中，第一溶液中油溶性聚合单体的质量分数为5％-90％。
进一步的，在步骤(2)中，第二溶液中聚合物的质量分数为5％-90％。
进一步的，在步骤(3)中，辐射发光单体为2，5-二苯基噁唑(PPO)、2-(4-联苯基)-5-苯基-1，3，4-噁二唑(PBD)和1，4-双(5-苯基-2-噁唑基)苯(POPOP)中的一种或几种。进一步的，在步骤(3)中，聚合物微球固体粉末与辐射发光单体在水中充分搅拌24h。
进一步的，在步骤(3)中，水溶性聚合单体为丙烯酰胺(AAM)和/或丙烯酸(AAC)。
进一步的，在步骤(3)中，第三溶液中聚合物微球固体粉末的质量分数为5％-90％，第三溶液中辐射发光单体的质量分数为0.02％-1.5％。
进一步的，在步骤(3)中，第四溶液中水溶性聚合单体的质量分数为5％-20％。
进一步的，在步骤(1)和步骤(4)中，γ射线源为钴源。
进一步的，在步骤(2)和步骤(4)中，辐照剂量率为2kGy/h，辐照交联时间为15h。
进一步的，用于放射治疗三维剂量验证的凝胶用于制备三维剂量验证的组织等效性辐射发光水凝胶剂量计。
借由上述方案，本发明具有以下优点：
本发明的用于放射治疗三维剂量验证的凝胶的制备方法，采用两步法，不仅合成方法快速简单，且成本低廉、产量大、无其他副产物；采用辐照交联法，不用掺杂其他试剂，使获得的凝胶更加纯净，且可以大批量制造；制备的凝胶具有良好的发光效率，保持透光性，机械强度高，且具有很好的组织等效性，便于本发明中的凝胶剂量计在临床放疗过程中的剂量验证。
上述说明仅是本发明技术方案的概述，为了能够更清楚了解本发明的技术手段，并可依照说明书的内容予以实施，以下以本发明的较佳实施例并配合附图详细说明如后。
附图说明
图1是本发明3D剂量验证的凝胶均匀网状结构截面SEM图；
图2是本发明3D剂量验证的凝胶截面局部放大SEM图。
具体实施方式
下面结合附图和实施例，对本发明的具体实施方式作进一步详细描述。以下实施例用于说明本发明，但不用来限制本发明的范围。
实施例1
取5ml的苯乙烯与95ml的去离子水混合，通入氮气除氧后，送入2kGy/h的钴源中辐照交联15h，得到聚苯乙烯微球溶液，1000转/分离心，冷冻干燥后得到聚苯乙烯微球粉末。将0.01g的聚苯乙烯微球与0.01g的PPO粉末在50ml的去离子水充分搅拌24h后，再与50ml溶解了5g丙烯酰胺的水溶液混合，通入氮气除氧后，送入2kGy/h的钴源中辐照交联15h，冷冻干燥48h后得到用于放射治疗三维剂量验证的凝胶。图1为3D剂量验证的凝胶均匀网状结构截面SEM图，可以看出，该凝胶具有均匀的网状结构，孔的大小均一，形貌完整。
图2为本发明3D剂量验证的凝胶截面局部放大SEM图，从图中可以看出凝胶网状结构表面凸起的结构，为凝胶剂量计的发光部分。
实施例2
取5ml的苯乙烯与95ml的去离子水混合，通入氮气除氧后，送入2kGy/h的钴源中辐照交联15h，得到聚苯乙烯微球溶液，1000转/分离心，冷冻干燥后得到聚苯乙烯微球粉末。将10g的聚苯乙烯微球与10g的PPO粉末在50ml的去离子水充分搅拌24h后，再与50ml溶解了20g的丙烯酰胺水溶液混合，通入氮气除氧后，送入2kGy/h的钴源中辐照交联15h，冷冻干燥后得到用于放射治疗三维剂量验证的凝胶。
实施例3
取5ml的苯乙烯与95ml的去离子水混合，通入氮气除氧后，送入2kGy/h的钴源中辐照交联15h，得到聚苯乙烯微球溶液，1000转/分离心，冷冻干燥后得到聚苯乙烯微球粉末。将0.01g的聚苯乙烯微球与0.01g的POPO粉末在50ml的去离子水充分搅拌24h后，再与30ml溶解了20g的丙烯酸水溶液混合，通入氮气除氧后，送入2kGy/h的钴源中辐照交联15h，冷冻干燥后得到用于放射治疗三维剂量验证的凝胶。
实施例4
取90ml的4-苯基-1-丁烯与10ml的去离子水混合，通入氮气除氧后，送入2kGy/h的钴源中辐照交联15h，得到聚4-苯基-1-丁烯微球溶液，1000转/分离心，冷冻干燥后得到聚4-苯基-1-丁烯微球粉末。将10g的聚4-苯基-1-丁烯微球与10g的POPOP粉末在50ml的去离子水充分搅拌24h后，再与45ml溶解了5g的丙烯酸水溶液混合，通入氮气除氧后，送入2kGy/h的钴源中辐照交联15h，冷冻干燥后得到用于放射治疗三维剂量验证的凝胶。
实施例5
取90ml的4-苯基-1-丁烯与95ml的去离子水混合，通入氮气除氧后，送入2kGy/h的钴源中辐照交联15h，得到聚4-苯基-1-丁烯微球溶液，100000转/分离心，冷冻干燥后得到聚4-苯基-1-丁烯微球粉末。将0.01g的聚4-苯基-1-丁烯微球、0.01g的PPO和0.01g的POPOP粉末在50ml的去离子水充分搅拌24h后，再与45ml溶解了5g的丙烯酸与5g的丙烯酰胺水溶液混合，通入氮气除氧后，送入2kGy/h的钴源中辐照交联15h，冷冻干燥后得到用于放射治疗三维剂量验证的凝胶。
以上所述仅是本发明的优选实施方式，并不用于限制本发明，应当指出，对于本技术领域的普通技术人员来说，在不脱离本发明技术原理的前提下，还可以做出若干改进和变型，这些改进和变型也应视为本发明的保护范围。
Claims (7)
1.一种用于放射治疗三维剂量验证的凝胶的制备方法，其特征在于，包括以下步骤：
(1)将油溶性聚合单体与水混合，得到第一溶液；所述油溶性聚合单体为苯乙烯、4-苯基-1-丁烯、烯丙苯、对甲基苯乙烯、间甲基苯乙烯、丙烯酸甲酯、丙烯酸丁酯和丙烯酸丙酯中的一种或几种；
(2)将步骤(1)中的所述第一溶液除氧，然后放入γ射线源中辐照交联，得到含有聚合物的第二溶液，离心，冷冻干燥，得到聚合物微球固体粉末；
(3)将步骤(2)得到的所述聚合物微球固体粉末与辐射发光单体在水中混合，得到第三溶液，将水溶性聚合单体溶于水中，得到第四溶液；所述辐射发光单体为2，5-二苯基噁唑、2-(4-联苯基)-5-苯基-1，3，4-噁二唑和1，4-双(5-苯基-2-噁唑基)苯中的一种或几种；所述水溶性单体为丙烯酸和/或丙烯酰胺；
(4)将步骤(3)中的所述第三溶液和第四溶液混合，除氧，然后放入γ射线源中辐照交联，得到所述用于放射治疗三维剂量验证的凝胶。
2.根据权利要求1所述的用于放射治疗三维剂量验证的凝胶的制备方法，其特征在于：在步骤(1)中，所述第一溶液中油溶性聚合单体的质量分数为5％-90％。
3.根据权利要求1所述的用于放射治疗三维剂量验证的凝胶的制备方法，其特征在于：在步骤(2)中，所述第二溶液中聚合物的质量分数为5％-90％。
4.根据权利要求1所述的用于放射治疗三维剂量验证的凝胶的制备方法，其特征在于：在步骤(3)中，所述第三溶液中聚合物微球固体粉末的质量分数为5％-90％，所述第三溶液中辐射发光单体的质量分数为0.02％-1.5％。
5.根据权利要求1所述的用于放射治疗三维剂量验证的凝胶的制备方法，其特征在于：在步骤(3)中，所述第四溶液中水溶性聚合单体的质量分数为5％-20％。
6.根据权利要求1所述的用于放射治疗三维剂量验证的凝胶的制备方法，其特征在于：在步骤(1)和步骤(4)中，所述γ射线源为钴源。
7.根据权利要求1-6任意一项权利要求所述的用于放射治疗三维剂量验证的凝胶，其特征在于：所述用于放射治疗三维剂量验证的凝胶在制备三维剂量验证的组织等效性辐射发光水凝胶剂量计中的应用。
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