CN107188533B - 一种地聚合物陶瓷固化高放废液的方法 - Google Patents
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Abstract
本发明公布了一种地聚合物陶瓷固化高放废液的方法,其实质是一种铝硅酸盐聚合物陶瓷固化核废液的方法。主要包括如下几个步骤:(1)无机吸附材料对高放废液中的核素进行吸附富集;(2)含核素吸附材料与无机固化剂,碱激发剂混合制备地聚合物基核废物中间固化体;(3)地聚合物核素固化体在热压条件下生成致密的地聚合物陶瓷固化体。该方法制备的地聚合物中间固化体性能稳定,便于暂存或运输。该方法核废液减容量大,最终的陶瓷固化体稳定性好,制备工艺简单,能耗低,无二次污染,易于工程化应用,可广泛用于高放废物的固化处理。
Description
技术领域
本发明涉及一种高放废液的处置方法,属于一种高放废液陶瓷固化处理技术与材料领域。
背景技术
随着能源消耗量的增加,化石能源储备急剧减少,核能作为一种新型的清洁能源被广泛应用。目前中低放废液的处理技术比较成熟,并成功用于生产实践,但高放废液的处理技术还有待发展。后处理高放废液汇聚了99%左右的放射性,具有放射时间长、核素毒性大和发热性等特点,引起了国内外学者的广泛关注。
高放废液的处理环节主要包括废液的预处理、废液固化、固化体的最终处置。高放废液煅烧浓缩处理温度高,能耗大,产生大量放射性气体,处理成本高。高放废液固化最常用的处理技术主要有:玻璃固化、陶瓷固化和水泥固化等。
玻璃固化工艺技术是将废物掺和在玻璃基料中形成玻璃固化体的过程。目前,玻璃固化高放废液技术已经在工程上实现了广泛应用。中国专利CN103265169A和中国专利CN101826376A中分别公布了固化原材料经高温熔融、成型退火后,制备出玻璃固化体的方法,该方法所得固化体依然存在耐辐射性能差、机械稳定性差、以及热稳定性差等缺点,且在高温和潮湿条件下,玻璃相会溶蚀、析晶,浸出率高,包容量低,不利于进行长期地质处置。
陶瓷固化工艺技术是将放射性核素与固化基材混合后经加压升温制备陶瓷固化体的过程。中国专利CN103408304B、CN101624267A和CN104844190A中分别利用铈独居石、拜耳法赤泥、氟磷灰石制备陶瓷固化体,所得固化体化学性能稳定,安全系数高,具有实际的工程应用潜力。玻璃陶瓷固化属于陶瓷固化的一种,中国专利CN104810072A和中国专利CN102568636A中使用不同原材料制备出的玻璃陶瓷固化体均具有较好的地质稳定性、化学稳定性、热稳定性和抗辐射性能,可以弥补玻璃固化的缺陷。
碱激发水泥新型胶凝材料也可实现对高放废液的固化。中国专利CN101261887A公布了一种碱矿渣水泥固化高放废液的方法,将高放废液经亚铁氰化镍钾预处理,碱化并与沸石、碱矿渣、激发剂混合,在一定水胶比下制备固化体。该技术利用沸石作为吸附剂,再对高放废液进行固化,具有良好的固化性能、较强的抗渗能力、以及较好的抗冲击性能,但该技术依然存在长期热稳定性较差等缺点。为了克服碱激发水泥固化的缺陷,本发明利用无机硅铝酸盐吸附剂吸附高放废液,再将含核吸附材料、无机固化剂以及碱激发剂混合制备地聚合物固化体,并在热压条件下将地聚合物固化体进一步致密化和高温陶瓷化。本发明中地聚合物固化过程无需添加任何有机添加剂,具有吸附-固化一体化的特性,进一步加压陶瓷化后,所得陶瓷固化体致密度高,具有较好的抗高温、耐辐照和抗浸出性能,可以弥补水泥固化的不足,且该技术工艺简单,能耗小,无二次污染,易于工程化应用。
发明内容
本发明提供了一种地聚合物陶瓷固化高放废液的方法,具体发明内容如下:
(1)本发明采用无机吸附材料富集高放废液中的核素,同时将含核吸附材料、固化剂和碱激发剂混合制备地聚合物中间固化体。无机吸附材料在碱激发剂作用下参与地聚合反应,既起到了吸附剂的作用,又起到了固化剂的作用;
(2)本发明对地聚合物中间固化体进一步致密化和高温陶瓷化,提升了最终核素固化体的抗高温、耐辐照和抗浸出性能。
本发明的有益效果:
(1)本发明原材料丰富,能耗低,工艺简单,易于工程应用;
(2)本发明不需添加任何有机添加剂,中间固化体不需要加压成型,可自行浇筑硬化;
(3)中间固化体可直接热压陶瓷化,不需任何其它添加剂,陶瓷固化体性能优良;
(4)本发明所涉及整个制备过程和使用过程无任何有毒有机污染物产生,安全环保。
具体实施方式
实施案例1:
一种地聚合物陶瓷固化高放废液的方法,以含锶沸石与偏高岭土质量比1:1混合,水玻璃模数1.5,碱灰比2:3,水灰比0.35制备地聚合物中间固化体,养护20d,抗压强度达48MPa。地聚合物固化体在真空热压烧结炉中1200°C,20MPa压力下,烧结6h得到地聚合物陶瓷固化体。固化体依据ASTM 标准中PCT 法对抗浸出性能进行分析,测得的28d 锶元素的标准化浸出率在10-5以下。
实施案例2:
一种地聚合物陶瓷固化高放废液的方法,以含锶沸石与偏高岭土质量比1:1混合,水玻璃模数1.2,碱灰比3:5,水灰比0.35制备地聚合物中间固化体,养护20d,抗压强度达45MPa。地聚合物固化体在真空热压烧结炉中1400℃,20MPa压力下,烧结6h得到地聚合物陶瓷固化体。固化体依据ASTM 标准中PCT 法对抗浸出性能进行分析,测得的28d 锶元素的标准化浸出率在10-5以下。
最后说明的是,以上优选实施例仅用以说明本发明的技术方案而非限制,尽管通过上述优选实施例已经对本发明进行了详细的描述,但本领域技术人员应当理解,可以在形式上和细节上对其做出各种各样改变,而不偏离本发明权利要求书所限定的范围。
Claims (6)
1.一种地聚合物陶瓷固化高放废液的方法,其主要特征在于,主要包括如下几个步骤:
(1)核素的富集:无机吸附材料对高放废液中的核素进行富集;
(2)地聚合物中间固化体的制备:步骤(1)中富集了核素的无机吸附材料与无机固化剂,碱激发剂混合,加水搅拌均匀,浇筑养护即得地聚合物中间固化体;
(3)地聚合物中间固化体高温陶瓷化:地聚合物中间固化体在热压条件下生成致密的地聚合物陶瓷固化体。
2.根据权利要求1中所述的一种地聚合物陶瓷固化高放废液的方法,其主要特征如下:无机吸附材料为无机硅铝酸盐吸附剂,主要包括沸石、膨润土、粘土、蒙脱石和埃洛石中的一种或几种。
3.根据权利要求1中所述的一种地聚合物陶瓷固化高放废液的方法,其主要特征如下:无机固化剂为具有火山灰特性的矿物或工业废渣,主要包括偏高岭土、粉煤灰、固硫灰、钢渣、高炉渣中的一种或几种。
4.根据权利要求1中所述的一种地聚合物陶瓷固化高放废液的方法,其主要特征如下:m固化剂:m吸附剂=0.25-4.0。
5.根据权利要求1中所述的一种地聚合物陶瓷固化高放废液的方法,其主要特征如下:高温陶瓷化在真空热压烧结炉或放电等离子体烧结炉中进行。
6.根据权利要求1中所述的一种地聚合物陶瓷固化高放废液的方法,其主要特征如下:热压条件为温度1200℃以上,压力20 MPa以上,烧结时间2h以上。
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CN104538076A (zh) * | 2014-12-02 | 2015-04-22 | 西南科技大学 | 一种放射性总活度-质量浓度梯度组合递降处理高中放废液的方法 |
JP2015231610A (ja) * | 2014-06-10 | 2015-12-24 | 国立大学法人山口大学 | 汚染水の処理方法 |
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EP0180308A1 (en) * | 1984-10-25 | 1986-05-07 | Mobil Oil Corporation | Borosilicate zeolite for nuclear waste disposal |
CN101261887A (zh) * | 2008-04-22 | 2008-09-10 | 南京瑞迪高新技术公司 | 用碱矿渣水泥固化高放废液的方法 |
JP2015231610A (ja) * | 2014-06-10 | 2015-12-24 | 国立大学法人山口大学 | 汚染水の処理方法 |
CN104282353A (zh) * | 2014-09-24 | 2015-01-14 | 深圳航天科技创新研究院 | 放射性蒸残液固化用的地质水泥及其固化方法 |
CN104538076A (zh) * | 2014-12-02 | 2015-04-22 | 西南科技大学 | 一种放射性总活度-质量浓度梯度组合递降处理高中放废液的方法 |
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