模拟高放玻璃固化体的析晶行为
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摘要
在高放废物玻璃熔制过程中,高放废物罐中心区域玻璃长时间处于高温状态,发生析晶现象。析晶增加了高放玻璃固化体的相界面,改变了其物理性质和化学性质。为了避免析晶的发生,必须研究高放玻璃固化体的析晶行为。本工作采用恒温热处理方式,研究模拟高放玻璃固化体的析晶行为。将模拟高放玻璃粉末分别在500、600、700、800、900℃下进行了0.5~96h的热处理。采用X射线衍射法(XRD)检测热处理后样品的结晶度和晶相。XRD测试结果表明:模拟高放玻璃固化体的最大结晶度析晶温度在700℃左右;热处理后产生了三类晶相辉石、斜长石和方铈矿,辉石出现在600~900℃,为主要晶相,方铈矿出现在700~900℃,斜长石只出现在700℃。
In the production process of high-level waste(HLW)glass,there was crystalline phase in the centre area of the HLW glass tanks,due to high temperature.Crystallization increases phase interface of HLW glass,having an effect on the physical and chemical properties of HLW glass.In order to avoid the occurrence of crystallization,it's necessary to study the crystallization behavior of HLW glass.Crystallization behaviors of the simulated HLW glass were researched by the isothermal heat treatment in this paper.The simulated HLW glass powders were respectively heated at 500,600,700,800,900℃in the range from 0.5hto 96 h.After heat treatment,the crystallinity and crystallinity phase of samples were detected by X-ray diffraction(XRD).The results of XRD show that the maximum degree of crystallinity of the simulated HLW glass appears at about 700℃.After isothermal heat treatment,there are three different crystals:omphacie,cerianite and albite.Omphacite is the major crystalline phase,which has always existed in the range from 600℃to 900℃.Cerianite always precipitates in the range from 700℃ to 900℃.Albite only precipitates at 700℃.
In the production process of high-level waste(HLW)glass,there was crystalline phase in the centre area of the HLW glass tanks,due to high temperature.Crystallization increases phase interface of HLW glass,having an effect on the physical and chemical properties of HLW glass.In order to avoid the occurrence of crystallization,it's necessary to study the crystallization behavior of HLW glass.Crystallization behaviors of the simulated HLW glass were researched by the isothermal heat treatment in this paper.The simulated HLW glass powders were respectively heated at 500,600,700,800,900℃in the range from 0.5hto 96 h.After heat treatment,the crystallinity and crystallinity phase of samples were detected by X-ray diffraction(XRD).The results of XRD show that the maximum degree of crystallinity of the simulated HLW glass appears at about 700℃.After isothermal heat treatment,there are three different crystals:omphacie,cerianite and albite.Omphacite is the major crystalline phase,which has always existed in the range from 600℃to 900℃.Cerianite always precipitates in the range from 700℃ to 900℃.Albite only precipitates at 700℃.
引文
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[10]王孝强,庹先国,周慧,等.高硫高钠高放废液玻璃固化配方研究[J].核化学与放射化学,2013,35(3):180-192.
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[12]Turcotte R P,Wald J W.Devitrification behavior in a zinc borosilicate nuclear waste glass,PNL-2247[R].Richland,Washington:Battelle Pacific Northwest Labs,1978.
[13]Cicero C A,Marra S L,Andrews M K.Phase stability determinations of DWPF waste glasses(U),WSRC-TR-93-00227[R].Aiken:Westinghouse Savannah River Company,1993.
[2]Matyas J,Huckleberry A R,Rodriguez C P,et al.HLW glass studies:development of crystal-tolerant HLW glasses,PNNL-21308[R].Richland,Washington:Pacific Northwest National Laboratory(PNNL),2012.
[3]Riley B J,Rosario J A,Hrma P.Impact of HLW glass crystallinity on the PCT response,PNNL-13491[R].Richland,Washington:Pacific Northwest National Laboratory,2001.
[4]Fox K M,Edwars T B,Peeler D K,et al.Durability and nepheline crystallization study for high level waste(HLW)sludge BATCH4(SB4)glasses formulated with Frit 503,WSRC-STI-2006-00009[R].Aiken,SC29808:Savannah River National Laboratory,2006.
[5]许嗣坤,柳得橹.模拟玻璃固化体析晶影响的研究[J].核科学与工程,1995,15(3):284-288.
[6]罗上庚,姜耀中,柳得橹.模拟高放废物玻璃固化体的析晶行为研究[J].核科学与工程,1990,10(2):154-159.
[7]Amoroso J.The impact of kinetics on nepheline formation in nuclear waste glasse,SRNL-STI-2011-00051[R].LLC Aiken,SC 29808:Savannah River Nuclear Solutions,2011.
[8]Donald I W,Metcalfe B L,Taylor R N J.The immobilization of high level radioactive wastes using ceramics and glasses[J].J Mater Sci,1997,32:5851-5887.
[9]罗上庚.放射性废物处理与处置[M].北京:中国环境科学出版社,2006:127-128.
[10]王孝强,庹先国,周慧,等.高硫高钠高放废液玻璃固化配方研究[J].核化学与放射化学,2013,35(3):180-192.
[11]赵彦钊,殷海荣.玻璃工艺学[M].北京:化学工业出版杜,1987:70.
[12]Turcotte R P,Wald J W.Devitrification behavior in a zinc borosilicate nuclear waste glass,PNL-2247[R].Richland,Washington:Battelle Pacific Northwest Labs,1978.
[13]Cicero C A,Marra S L,Andrews M K.Phase stability determinations of DWPF waste glasses(U),WSRC-TR-93-00227[R].Aiken:Westinghouse Savannah River Company,1993.