鐵磷酸鹽玻璃陶瓷固化體結(jié)構(gòu)與化學(xué)穩(wěn)定性的研究
發(fā)布時間:2018-07-12 16:04
本文選題:玻璃陶瓷 + 二氧化鈦 ; 參考:《西南科技大學(xué)》2015年碩士論文
【摘要】:獨居石鐵磷酸鹽玻璃陶瓷固化兼具鐵磷酸鹽玻璃固化和獨居石陶瓷固化的優(yōu)點,是最新一代高放廢物固化方法。本文以36Fe2O3-54P2O5-10Ca F2為基礎(chǔ)玻璃,先分別摻入Ti O2和Ba O改善玻璃基體的性能,再經(jīng)過析晶熱處理制備出具有優(yōu)良化學(xué)穩(wěn)定性的獨居石鐵磷酸鹽玻璃陶瓷固化體,利用XRD、SEM-EDS、FTIR等現(xiàn)代分析測試方法對樣品的結(jié)構(gòu)特點和表面形貌進(jìn)行分析表征,通過MCC-1靜態(tài)浸出實驗研究玻璃陶瓷固化體樣品的化學(xué)穩(wěn)定性,得到如下主要結(jié)論:(1)基礎(chǔ)鐵磷酸玻璃的摻雜改性:XRD分析表明,鋇鐵磷酸鹽玻璃在650~850℃析晶熱處理時,析出的主晶相為Fe PO4,且Ba O的摻量增加會抑制Fe PO4的析出。FTIR及Raman光譜分析表明:兩個體系的鐵磷酸鹽玻璃具有相似的結(jié)構(gòu),均以Q1結(jié)構(gòu)單元為主,DTA測試結(jié)果表明,Ti O2可以增強玻璃結(jié)構(gòu)的內(nèi)聚力,增強熱穩(wěn)定性。Ba O作為一種網(wǎng)絡(luò)修飾體,適量時可以改善玻璃的熱穩(wěn)定性,Ti O2的加入可以增大玻璃密度。(2)獨居石鐵磷酸鹽玻璃陶瓷固化體:鐵鈦磷酸鹽玻璃陶瓷固化體的主晶相和次晶相分別為獨居石和Fe9Ti O15,樣品T15-50W的析晶效果較佳,玻璃相的主要成分為Al PO4.鐵鋇磷酸鹽玻璃陶瓷固化體中,Ba O可以抑制獨居石的析出,當(dāng)Ba O的摻量達(dá)到20mol%時,固化體又析出了Zr P2O7和Ba Al2Si2O8等雜相。FTIR分析表明,兩個體系的玻璃陶瓷固化體吸收峰的位置也基本一致,且隨著Ti O2和Ba O含量的增大,Q1和Q2基團的特征吸收峰強度逐漸減弱,Q0基團的吸收峰卻明顯增強。密度測試說明,二氧化鈦可以促進(jìn)玻璃析晶,使固化體結(jié)構(gòu)更加致密化,而固化體樣品的密度隨氧化鋇含量加入先增大后減小;瘜W(xué)穩(wěn)定性實驗表明:兩個體系的固化體試樣的浸出率都隨著時間的延長逐漸下降,14天前下降較快,14天到28天期間緩慢下降,28天以后逐漸趨于穩(wěn)定,最后達(dá)到平衡。鐵鈦磷酸鹽玻璃陶瓷固化體質(zhì)量損失速率數(shù)量級都在10-10~10-9 g/cm2·min,溶液中大部分離子的浸出率都接近或低于儀器檢出限,表明鐵鈦磷酸鹽玻璃陶瓷固化體試樣具有極強的化學(xué)穩(wěn)定性。鐵鋇磷酸鹽玻璃陶瓷固化體的的質(zhì)量損失速率數(shù)量級在10-8~10-9 g/cm2·min。
[Abstract]:The solidification of monazite iron phosphate glass ceramic has the advantages of both iron phosphate glass curing and monazite ceramic curing. It is the latest generation of high-level waste curing method. In this paper, based on 36Fe _ 2O _ 3-54P _ 2O _ 5-10Ca _ F _ 2 glass, the properties of glass matrix were improved by adding TIO _ 2 and Ba _ O respectively, then the monazite iron-phosphate glass ceramics with excellent chemical stability were prepared by crystallization heat treatment. The structure and surface morphology of the samples were analyzed and characterized by means of modern analysis and FTIR, such as XRDX SEM-EDSX FTIR. The chemical stability of the glass-ceramic solidified samples was studied by static leaching experiments of MCC-1. The main conclusions are as follows: (1) the doping modification of the base iron-phosphate glass shows that the barium ferric phosphate glass is crystallized at 650 ~ 850 鈩,
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