Pressureless in-situ synthesis of MgAlON composites from spent slide bricks and spent MgO-C bricks

doi:10.3969/j.issn.1001-1935.2024.06.009

Abstract

Abstract: To analyze whether sintered chrome-corundum materials meet the requirements of the corrosion resistance of ceramic electric melting furnaces against borosilicate glass,the corrosion behaviours of simulated high level radioactive liquid waste vitrified glass to two sintered chrome-corundum refractories with different Cr₂O₃ contents (47.3% and 60.9%,by mass) at 1 200 ℃ through the rotary impregnation method were compared and investigated.The microstructure and phase composition of the two chrome-corundum refractories after the corrosion tests were analyzed.The results indicate that:(1)the sintered chrome-corundum refractories exhibit excellent corrosion resistance against the simulated molten glass,while showing a discontinuous corrosion process of matrix corrosion-grain spalling;(2) molten glass mainly infiltrates through the pores and phosphate phases between (Cr,Al)₂O₃ solid solution in the sintered chrome-corundum refractories;whereas Al₂O₃ of (Cr,Al)₂O₃ solid solution diffuses into the molten glass,and MgO,FeO,Fe₂O₃,etc. diffuse from the molten glass into (Cr,Al)₂O₃ solid solution,forming Al₂O₃-poor composite spinel;(3)the sample with 60.9% Cr₂O₃ has slightly worse corrosion resistance than the one with 47.3% Cr₂O₃,because the poor solid solubility of (Cr,Al)₂O₃ solid solution,and the poor direct bonding of phosphate binders and (Cr,Al)₂O₃ solid solution matrix with Al₂O₃ as well as Cr₂O₃ particles worsen the corrosion resistance of the sample;(4)if the bonding strength between matrix and particles of sintered chrome-corundum refractories is enhanced,forming similar structures as fused materials,the problem of discontinuous corrosion in molten glass will be solved,the corrosion resistance against molten glass will be improved,and the refractories are potential to be applied in ceramic electric melting furnaces.

Key words: ceramic electric melting furnaces, sintered chrome-corundum, simulated high level radioactive liquid waste vitrified glass, corrosion resistance

摘要： 为了分析烧结铬刚玉材料是否符合陶瓷电熔炉对硼硅酸盐玻璃抗侵蚀性能的要求,采用旋转浸渍法对比研究了1 200 ℃下模拟高放废液固化玻璃液对2种Cr₂O₃含量(Cr₂O₃的质量分数分别为47.3%和60.9%)的烧结铬刚玉材料的侵蚀行为,并分析了侵蚀试验后的2种烧结铬刚玉材料的显微结构和物相组成。结果表明:1)烧结铬刚玉抗模拟玻璃液侵蚀性优异,但烧结铬刚玉材料在玻璃液中的动态侵蚀过程为基质侵蚀-颗粒剥落的非连续蚀损。2)玻璃液在烧结铬刚玉中的渗透主要表现为沿材料气孔及(Cr,Al)₂O₃固溶体间磷酸盐相向内渗透;(Cr,Al)₂O₃固溶体中的Al₂O₃扩散进入玻璃液中,玻璃液中的MgO、FeO和Fe₂O₃等扩散进入 (Cr,Al)₂O₃ 固溶体,形成贫Al₂O₃的复合尖晶石。3)含60.9%(w)Cr₂O₃的试样对硼硅酸盐的抗侵蚀性较含47.3%(w)Cr₂O₃试样的略差,原因是含60.9%(w)Cr₂O₃的试样中(Cr,Al)₂O₃固溶体固溶度低,磷酸盐结合剂以及(Cr,Al)₂O₃固溶体基质与Al₂O₃和Cr₂O₃颗粒的直接结合程度差,均对其抗侵蚀性产生了不利影响。4)烧结铬刚玉材料若提高基质与颗粒间的结合强度,形成类电熔材料结构特征,改善其在玻璃液中的不连续蚀损问题,提高烧结铬刚玉材料抗玻璃液侵蚀能力,则有望在陶瓷电熔炉上应用。

关键词: 陶瓷电熔炉, 烧结铬刚玉, 模拟高放废液固化玻璃, 抗侵蚀性

CLC Number:

TQ175

付琪琪, 赵庆彬, 张利新, 邓俊杰, 何旭辉, 陈留刚. 烧结铬刚玉在陶瓷电熔炉中应用的可行性研究[J]. 耐火材料, 2024, 58(6): 506-512.

References

[1] 张威,董海龙,阮苠秩.陶瓷电熔炉在动力堆高放废液玻璃固化中适用性分析[J].辐射防护,2019,39(4):322-330.
[2] 凡思军,钱敏,薛天锋,等.Joule加热陶瓷炉玻璃固化技术研究进展[J].硅酸盐学报,2021,49(12):2736-2750.
[3] 李玉松,张生栋,鲜亮,等.CIAE高放废液固化技术研发进展[J].原子能科学技术,2020,54(S1):126-136.
[4] 徐凯.核废料玻璃固化国际研究进展[J].中国材料进展,2016,35(7):481-517.
[5] 刘丽君.我国高放废液玻璃固化技术四十年的发展[C]//中国核学会2015年学术年会论文集,绵阳,2015(4):389-393.
[6] 傅茂洋.含镧硼硅酸盐玻璃及玻璃陶瓷结构和性能的研究[D].绵阳:西南科技大学,2023.
[7] 钱敏,凡思军,薛天锋,等.高放废液硼硅酸盐玻璃固化配方研究进展[J].硅酸盐学报,2021,49(10):2251-2265.
[8] 董海龙,梁璇,姚美玲.高放废液中放射性铯的玻璃固化配方研究[J].广东化工,2024,51(7):52-54.
[9] 徐卫东.浅析高放废液玻璃固化技术[J].中国建材科技,2022,31(3):65-69.
[10] 郑宇,张辉,潘亚兰,等.高放废液玻璃陶瓷固化电熔炉耐火内衬材料选择及熔炉构型初步设计[J].原子能科学技术,2021,55(S1):30-36.
[11] JIN T,HALL M,VIENNA J,et al.Glass-contact refractory of the nuclear waste vitrification melters in the United States:a review of corrosion data and melter life[J].International Materials Reviews,2023,68(8):1135-1157.
[12] 孙红刚,李红霞,杜一昊,等.三种渣对危废焚烧回转窑用镁尖晶石砖和铬刚玉砖的侵蚀试验[J].耐火材料,2020,54(6):518-521.
[13] 王相辉.冶金渣对铬刚玉质耐火材料的侵蚀性研究[D].武汉:武汉科技大学,2019.
[14] 柯昌明,李有奇,赵继增,等.水煤浆气化炉用高铬耐火材料的研究进展[J].耐火材料,2014,48(4):298-301.
[15] 李红霞,孙红刚.煤气化技术用耐火材料及发展趋势[J].耐火材料,2018,52(2):81-88.
[16] 王晗,李宏,吕诗宏,等.大尺寸铬刚玉砖烧结中温度场和应力场的分析[J].耐火材料,2019,53(2):137-140.
[17] 康鑫,张利新,邓俊杰,等.Cr₂O₃微粉加入量对Al₂O₃-Cr₂O₃质耐火材料性能的影响[J].硅酸盐通报,2021,40(10):3285-3291.
[18] SELKREGG K.Fusion cast refractories:Roles of containment[J].American Ceramic Society Bulletin,2018,97(2):21-28.
[19] XU X Y,SAINI R ,KORAY AKDOGAN E ,et al.Corrosion behavior of Monofrax K-3 refractory in borosilicate-based model low activity waste glass melts[J].Journal of the American Ceramic Society,2023,106(6):3375-3395.