| 183 | 3 | 32 |
| 下载次数 | 被引频次 | 阅读次数 |
以钕和铈作为放射性铀和钚的模拟核素,采用碱激发和水热法制备了模拟中放α废液"碱-矿渣-粉煤灰-煅烧高岭土"水合陶瓷固化体。研究了固化体的结构组成、力学性能、抗侵蚀性和化学稳定性。结果表明:固化体的主要晶相组成为方沸石和NaPl沸石;在水热条件下,固化体中掺入模拟中放α废液后有利于沸石晶相的形成。抗压强度测试表明,固化体中废物包容量达到40%左右时仍能满足水泥固化体抗压强度的要求。固化体经硫酸盐介质和地下水侵蚀28 d后,其抗压强度损失较少,外观没有裂纹和龟裂,说明固化体具有较好的的抗硫酸盐和地下水侵蚀性能。另外,静态浸出测试结果表明,Nd和Ce的浸出率在10-8~10-6cm/d范围,说明固化体具有优良的化学稳定性。
Abstract:The "alkali-activated slag-fly ash-calcined kaolin" hydroceramic(ASFCH) used for solidifying simulated medium level alpha liquid waste(S-MLALW) was prepared by alkaline activation and hydrothermal methods with neodymium and cerium as simulated radioactive nuclides of uranium and plutonium.The phase composition,mechanical strength,corrosion resistance and chemical stability of ASFCH waste forms were investigated.The results show that the main crystalline phase components of ASFCH waste forms are analcime and zeolite NaPl.The introduction of S-MLALW is contributed to the formation of zeolite phases in ASFCH waste form.According to the results of the compressive strength tests,the strength of ASFCH waste form still meets the requirement of cemented waste form when the waste package capacity is 40%.Moreover,the compressive strength of ASFCH waste forms decreases slightly after corrosion by sulphate solution and simulated ground water for 28 d.Also,there are no cracks and fractures appeared on the ASFCH waste forms.It is indicated that ASFCH waste form has a preferable corrosion resistance to sulphate solution and ground water.Besides,the leaching rates of neodymium and cerium are in the range of 10-8-10-6 cm/d,showing that ASFCH waste forms for solidifying S-MLALW also possesses superior chemical stability.
[1]顾忠茂.核废物处理技术[M].北京:原子能出版社,2009:9.
[2]王旭东.核设施退役与环境整治中α废物的最少化[J].辐射防护通讯,2003,23(5):13-15.
[3]胡曙光,陈袁魁,徐光亮,等.特种水泥(第二版)[M].武汉:武汉理工大学出版社,2010:184.
[4]SIEMER D D.Hydroceramics,a"new"cementitious waste form material for U.S defense-type reprocessing waste[J].Mater Res Innovations,2002,6(1):96-104.
[5]GRUTZECK M,KWAN S.Physical,chemical and structural evolution of zeolite-containing waste forms reproduced form metakaolin and calcined HLW[R].Department of Energy First Annual Report,PA,USA:University Park,2002,2-3;51-69.
[6]JOHNSON O.Hydroceramic transformation and dissolution of hydroceramic waste forms for the INNEL calcined high-level waste[D].Philadelphia,USA:The Pennsylvanian State University,2002.
[7]BAO Y Design and characterization of microporous zeolitic hydroceramic wastes for the solidification and stabilization of sodium bearing wastes[D].Philadelphia,USA:The Pennsylvanian State University,2005.
[8]CHEN Song,WU Mengqiang,ZHANG Shuren.Mineral phases and properties of alkali-activated metakaolin-slag hydroceramics for a disposal of simulated highly-alkaline wastes[J].J Nucl Mater,2010,402:173-178.
[9]WANG Jin,WU Xiuling,WANG Junxia,et al.Hydrothermal synthesis and characterization of alkali-activated slag-fly ash-metakaolin cementitious materials[J].Micropor Mesopor Mater,2012,155:186-191.
[10]王进,韩朝江,王军霞,等.“碱-矿渣-粉煤灰-偏高岭土”水合陶瓷产物组成和微观结构[J].硅酸盐学报,2011,39(3):512-517.WANG Jin,HAN Chaojiang,WANG Junxia,et al.J Chin Ceram Soc2011,39(3):512-517.
[11]PALOMO A,GRUTZECK M W,BLANCO M T.Alkali-activated fly ashes:a cement for the future[J].Cem Concr Res,1999,29:1323-1329.
[12]GRUTZECK M,KWAN S,DICOLA M.Zeolite formation in alkali-activated cementitious systems[J].Cem Concr Res,2004,34:949-955.
[13]BAO Y,GRUTZECK M W.Preparation and properties of hydroceramic waste forms made with simulated hanford low-activity waste[J].J Am Ceram Soc,2005,88(12):3287-3302.
[14]BAO Y,KWAN S.Binders for radioactive waste forms made from pretreated calcined sodium bearing waste[J].J Mater Sci,2004,2(39):481-488.
[15]王进,李林,王军霞,等.“碱-矿渣-粉煤灰-偏高岭土”水合陶瓷结构与性能[J].武汉理工大学学报,2011,33(2):27-31.WANG Jin,LI Lin,WANG Junxia,et al.J Wuhan Univ Technol(in Chinese),2011,33(2):27-31.
[16]梁俊福,宋崇立,潘翠玲,等.高放泥浆研究-模拟高放泥浆的配制及性能研究[J].核化学与放射化学,2000,22(1):37-44.LIANG Junfu,SONG Chongli,PAN Cuiling,et al.J Nucl Radiochem(in Chinese),2000,22(1):37-44.
[17]SHIRAHASHI K,KUBOTA M.Precipitation behavior of transuranium elements during denitration of high-level radioactive liquid waste by formic acid[J].J Nucl Sci Technol,1992,29(6):559-565.
[18]中华人民共和国国家质量监督检验检疫总局,中国国家标准化管理委员会.GB/T 749-2008水泥抗硫酸盐侵蚀试验方法[S].北京:中国标准出版社,2008.General Administration of Quality Supervision,Inspection and Quarantine of the People's Republic of China,Standardization Administration of China.GB/T 749-2008 Test method for determing capability of resisting sulfate corrode of cement(in Chinese).Beijing:Standards Press of China,2008.
[19]王金明,易发成.几种矿物材料对Cs~+吸附性能的研究[J].核化学与放射化学,2006,28(2):117-121.WANG Jinming,YI Facheng.J Nucl Radiochem(in Chinese),2006,28(2):117-121.
[20]国家环境保护局.GB7023-86放射性废物固化体长期浸出试验[S].北京:中国标准出版社,1986.State Environmental Protection Administration of China.GB7023-86Long-term leach testing of solidified radioactive waste forms(in Chinese).Beijing:Standards Press of China,1986.
[21]QUEROL X,MORENO N,UMANA J C,et al.Synthesis of zeolites from coal fly ash:an overview[J].Int J Coal Geol,2002,50:413-423.
[22]环境保护部,国家质量监督检验检疫总局.GB 14569.1-2011低、中水平放射性废物固化体性能要求-水泥固化体[S].北京:中国标准出版社,2011.Ministry of Environment Protection,General Administration of Quality Supervision,Inspection and Quarantine of the People's Republic of China,GB 14569.1-2011 Performance requirements for low and intermediate level radioactive waste form-Cemented waste form(in Chinese).Beijing:Standards Press of China,2011.
基本信息:
DOI:10.14062/j.issn.0454-5648.2015.04.04
中图分类号:TQ174.75;TL941.1
引用信息:
[1]王进,王军霞,雍超,等.“碱-矿渣-粉煤灰-煅烧高岭土”水合陶瓷固化模拟中放α废液[J].硅酸盐学报,2015,43(04):386-392.DOI:10.14062/j.issn.0454-5648.2015.04.04.
基金信息:
四川省非金属复合与功能材料重点实验室-省部共建国家重点实验室培育基地开放基金资助项目(11zxfk04,11zxfk26);; 西南科技大学博士基金(13zx7105)资助项目
2014-08-07
2014
2015-03-15
2014-10-14
2014
1
2015-04-15
2015-04-15