摘要
以Nd(Ⅲ)作为放射性核素An(Ⅲ)的模拟替代物,以Gd_2O_3和ZrO_2粉体为原料,通过高温固相反应法(1500℃,保温72 h)合成了Gd_(2-x)Nd_xZr_2O_7(0≤x≤2.0)微米级的钆锆烧绿石固化An(Ⅲ)的模拟固化体.利用X射线衍射仪、显微硬度计和扫描电子显微镜等对所制备样品的物相、密度、维氏硬度和微观形貌进行了表征.结果表明:Gd_(2-x)Nd_xZr_2O_7(0≤x≤2.0)系列固化体样品多呈板状,均为烧绿石相;其密度值随固溶量x值的增加,呈逐渐下降趋势,但均≥5.76 g·cm~(-3).固化体的维氏硬度值(H_v)随x值的递增呈逐渐减小趋势,x值与维氏硬度值之间满足H_v=695.18636-162.64091 x的线性关系,但维氏硬度值均≥400kg·mm~(-2)以上.
In order to investigate the capability of Gd_2Zr_2O_7 pyrochlore as a waste form for immobilizing trivalent actinides nuclides,Nd(Ⅲ) is used as an alternative substance for An(Ⅲ).The compounds in the system Gd_(2-x)Nd_xZr_2O_7(0≤x≤2.0) are synthesized at 1500℃for 72 h by high temperature solid state reaction method,using Gd_2O_3 and ZrO_2 powders as the raw materials.The phase, intensity,Vickers hardness and microcosmic shape are characterized by X-ray diffraction,Vickers hardness tester,scanning electron microscopy and so on.The results indicate mat the phase of synthesized waste form with plate-shape keeps the phase of pyrochlore. The intensity of compound slightly decreases with the increase of the containment capacity value x,but it is above 5.76 g·cm~(-3). The value of Vickers hardness also decreases with the increase of x.The values of x and Vickers hardness are linearly related by H_V = 695.18636 - 162.64091 x(H_V≥400 kg·mm~(-2)).
引文
[1]Amin Y M 1989 Nucl.Instrum.Methods Phys.Res.280 314
[2]Nasdala L,Irmer G,Wolf D 1995 Eur.J.Mineral.7 471
[3]Weber W J 1991 Radiation Effects and Defects in Solids 115 341
[4]Clarke D R 1983 Ann.Rev.Mater.Sci.13 191
[5]Robert L E J 1990 Annu.Rev.Part.Sci.40 79
[6]Wang S X,Begg B D,Wang L M,Ewing R C,Weber W J,Govidan Kutty K V 1999 J.Mater.Res.14 4470
[7]Weber W J,Ewing R C 2000 Science 289 2051
[8]Sickafus K E,Minervini L,Grimes R W 2000 Science 289 748
[9]Ewing R C,Weber W J,Lian J 2004 J.Appl.Phys.95 5949
[10]Chen J,Lian J,Wang L M,Ewing R C 2001 Appt.Phys.Lett.79 1989
[11]Lian J,Wang L M,Chen J,Sun K,Ewing R C,Farmer J M,Boatner L A 2003 Acta Mater.51 1493
[12]Lian J,Wang L M,Haire R G,Helean K B,Ewing R C 2004 Nucl. Instrum.Methods Phys.Res.B 218 236
[13]Lian J,Ewing R C,Wang L M,Helean K B 2004 J.Mater.Res. 19 1575
[14]Zhang F X,Lian J,Zhang J M,Moreno K J,Fuentes A F,Wang Z W,Ewing R C 2010 Journal of Alloy and Compounds 494 34
[15]Pan ZL 1993 Crystallography and Mineralogy(Vol.1)(Beijing: Geology Press) pl52(in Chinese)[潘兆鲁1993结晶学及矿物学(上)(北京:地质出版社)第152页]