Ca(OH)2注浆对碱激发固化铀尾矿渣性能的影响

doi:10.16085/j.issn.1000-6613.2023-1755

化工进展 ›› 2024, Vol. 43 ›› Issue (11): 6458-6467.DOI: 10.16085/j.issn.1000-6613.2023-1755

• 资源与环境化工 • 上一篇

Ca(OH)₂注浆对碱激发固化铀尾矿渣性能的影响

牛前进¹(), 李春光¹^,²^,³(), 刘振中¹^,², 刘龙成²^,⁴

^1.南华大学资源环境与安全工程学院，湖南衡阳 421001
^2.南华大学放射性废物处理处置与数学模型研发中心，湖南衡阳 421001
^3.中国原子能科学研究院，北京 102413
^4.核工业北京化工冶金研究院，北京 101121

收稿日期:2023-10-08 修回日期:2024-03-20 出版日期:2024-11-15 发布日期:2024-12-07
通讯作者: 李春光
作者简介:牛前进（1989—），男，硕士，研究方向为铀资源与环境。E-mail：1414239706@qq.com。
基金资助:
湖南省自然科学基金(2019JJ50496);湖南省教育厅科学研究优秀青年项目(20B494)

Effect of Ca(OH)₂ grouting on the property of alkali-activated solidified uranium tailing slags

NIU Qianjin¹(), LI Chunguang¹^,²^,³(), LIU Zhenzhong¹^,², LIU Longcheng²^,⁴

^1.School of Resource Environment and Safety Engineering, University of South China, Hengyang 421001, Hunan, China
^2.R&D Center of Radioactive Waste Treatment, Disposal and Modeling, University of South China, Hengyang 421001, Hunan, China
^3.China Institute of Atomic Energy, Beijing 102413, China
^4.Beijing Institute of Chemical and Metallurgy for Nuclear Industry, Beijing 101121, China

Received:2023-10-08 Revised:2024-03-20 Online:2024-11-15 Published:2024-12-07
Contact: LI Chunguang

摘要/Abstract

摘要：

铀尾矿库体积庞大、铀矿渣颗粒松散，具有潜在的溃坝和放射性污染扩散的风险。为了解决上述问题，采用Ca(OH)₂注浆与氢氧化钠-偏高岭土-水玻璃相结合的方法固化花岗岩型铀尾矿，研究注入不同质量分数的Ca(OH)₂对碱激发固化花岗岩型铀尾矿渣抗压强度、铀浸出性、氡析出性的影响规律，并进行微观形貌和理化分析，揭示其固化机制。实验结果表明：铀矿渣样品在注入Ca(OH)₂质量分数为15.0%，养护28天时其标准三轴抗压强度达到6.8MPa，与未注入Ca(OH)₂的样品相比强度提升4.4倍，铀浸出率下降89%，氡析出率降低52%。SEM和XRD分析表明，注入Ca(OH)₂质量分数为15.0%的试样与对照组试样相比，其内部形成了较多的C-S-H和C-A-H凝胶以及C-A-S-H聚合物，促进了铀尾矿渣固化抗压强度的提升，降低了铀浸出率和氡析出率。研究结果为碱激发在花岗岩型铀尾矿渣加固中应用奠定一定的理论基础。

关键词: 铀尾矿渣, 污染, 凝胶, 碱激发, 固定化, 铀浸出率, 氡析出率

Abstract:

The uranium tailings pond has a large volume and loose uranium tailing slags, which pose the risk of dam failure and diffusion of radioactive contamination. To address these issues, Ca(OH)₂ grouting combined with sodium hydroxide and metacolinite-water glass was utilized to solidify granite-type uranium tailing slags. The impact of injected Ca(OH)₂ mass fraction on the compressive strength, uranium leaching and radon exhalation of alkali-activated granite-type uranium tailings was investigated through microscopic morphology and physical and chemical analysis. Additionally, the solidification mechanism was elucidated. The experimental results showed that when the uranium slag was injected with 15.0% Ca(OH)₂, the standard triaxial compressive strength reached 6.8MPa after curing for 28d, which was a significant improvement of 4.4 times compared to the sample without Ca(OH)₂ injection. Additionally, adding Ca(OH)₂ reduced uranium leaching rate by 89% and radon exfiltration rate by 52%. SEM and XRD analysis indicated that compared with the control group, more gels of C-S-H and C-A-H and polymers of C-A-S-H were formed in the sample with Ca(OH)₂ mass fraction of 15.0%, which was the dominent reason for the improvement of compressive strength of solidified uranium tailing slags and the decrease of uranium leaching and radon exhalation. The research results laid a theoretical foundation for the application of alkali excitation in the reinforcement of granite-type uranium tailing slags.

Key words: uranium tailing slags, contamination, gels, alkali-activation, immobilization, uranium leaching rate, radon exhalation rate

中图分类号:

TL941⁺.33

牛前进, 李春光, 刘振中, 刘龙成. Ca(OH)₂注浆对碱激发固化铀尾矿渣性能的影响[J]. 化工进展, 2024, 43(11): 6458-6467.

NIU Qianjin, LI Chunguang, LIU Zhenzhong, LIU Longcheng. Effect of Ca(OH)₂ grouting on the property of alkali-activated solidified uranium tailing slags[J]. Chemical Industry and Engineering Progress, 2024, 43(11): 6458-6467.

图/表 18

图1 铀尾矿渣的颗粒级配曲线

表1 铀尾矿化学组成分析结果

组分	质量分数/%
SiO₂	85.25
Fe₂O₃	1.63
Al₂O₃	6.18
U	0.01
其他	6.85

表2 偏高岭土化学组成成分

组分	质量分数/%
SiO₂	54.28
Fe₂O₃	0.82
Al₂O₃	44.52
其他	0.38

表3 水玻璃化学组成成分

组分	质量分数/%
SiO₂	27.3
Na₂O	8.54
Be(20℃)	38.5

表4 固化铀尾矿各物质掺入量

组分	质量/g
铀尾矿	200
偏高岭土	54
NaOH	35
减水剂	2
水玻璃	32

图2 试样制备过程

图3 应力应变关系曲线

图4 相同养护时间不同Ca(OH)2注入量样品的XRD图谱

图5 未注入Ca(OH)2铀尾矿固化体SEM形貌图（28d）

图6 注入Ca(OH)2质量分数15%铀尾矿固化体SEM形貌图（28d）

图7 注入Ca(OH)2质量分数20%铀尾矿固化体SEM形貌图（28d）

图8 固化体凝胶物质EDS图谱结果

图9 随Ca(OH)2变化的铀浓度

图10 累积氡浓度

图11 各试样单面氡析出率值

图12 养护28天不同Ca(OH)2注入量样品图像

表5 Ca(OH)2注入量与孔隙率关系

Ca(OH)₂质量分数/%	孔隙率/%
0	16
5	10
10	8.8
15	0.95
20	1.2
25	4.6

图13 15% Ca(OH)2注入量样品养护28d XPS图谱

参考文献 28

1	TAN Kaixuan, LIU Zehua, XIA Liangshu, et al. The influence of fractal size distribution of covers on radon exhalation from uranium mill tailings[J]. Radiation Measurements, 2012, 47(2): 163-167.
2	LI Guangyue, HU Nan, DING Dexin, et al. Screening of plant species for phytoremediation of uranium, thorium, barium nickel, strontium and lead contaminated soils from a uranium mill tailings repository in South China[J]. Bulletin of Environmental Contamination and Toxicology, 2011, 86(6): 646-652.
3	STOJANOVIĆ Mirjana D, MIHAJLOVIĆ Marija L, MILOJKOVIĆ Jelena V, et al. Efficient phytoremediation of uranium mine tailings by tobacco[J]. Environmental Chemistry Letters, 2012, 10(4): 377-381.
4	姚凯, 李青, 王鹏淮, 等. 硬脂酸钠对碱激发矿渣-赤泥胶凝材料吸水速率的影响[J]. 硅酸盐通报, 2023, 42(5): 1778-1784, 1803.
	YAO Kai, LI Qing, WANG Penghuai, et al. Effect of sodium stearate on water absorption rate of alkali-activated slag-red mud cementitious material[J]. Bulletin of the Chinese Ceramic Society, 2023, 42(5): 1778-1784, 1803.
5	NAVARRO-BLASCO I, DURAN A, SIRERA R, et al. Solidification/stabilization of toxic metals in calcium aluminate cement matrices[J]. Journal of Hazardous Materials, 2013, 260: 89-103.
6	匡雅, 邹树梁, 徐立国, 等. 搅拌参数对放射性废液水泥固化体性能的影响[J]. 原子能科学技术, 2019, 53(2): 234-242.
	KUANG Ya, ZOU Shuliang, XU Liguo, et al. Effect of mixing parameter on property of cement solidified radioactive waste form[J]. Atomic Energy Science and Technology, 2019, 53(2): 234-242.
7	JIANG Fuliang, WANG Zhe, CHEN Guan, et al. Experimental study of pore characteristics and radon exhalation of uranium tailing solidified bodies in acidic environments[J]. Environmental Science and Pollution Research, 2021, 28(16): 20111-20120.
8	王亚超. 碱激发粉煤灰基地质聚合物强化增韧及耐久性能研究[D]. 西安: 西安建筑科技大学, 2014.
	WANG Yachao. Investigations on reinforcing, toughening and durability of alkali-activated fly ash-based geopolymer[D]. Xi’an: Xi’an University of Architecture and Technology, 2014.
9	王玲玲, 司晨玉, 李畅, 等. 氢氧化钾-钠水玻璃激发剂对碱激发矿渣胶凝材料性能的影响[J]. 硅酸盐通报, 2022, 41(8): 2654-2662.
	WANG Lingling, SI Chenyu, LI Chang, et al. Effect of potassium hydroxide-sodium water glass activator on properties of alkali-activated slag cementitious materials[J]. Bulletin of the Chinese Ceramic Society, 2022, 41(8): 2654-2662.
10	叶家元, 张文生, 史迪. 钙对碱激发胶凝材料的促凝增强作用[J]. 硅酸盐学报, 2017, 45(8): 1101-1112.
	YE Jiayuan, ZHANG Wensheng, SHI Di. Setting acceleration and strength enhancement derived from calcium species for alkali-activated cementitious materials[J]. Journal of the Chinese Ceramic Society, 2017, 45(8): 1101-1112.
11	袁正平, 耿新洋, 王富林. 碱激发冶炼铅渣-偏高岭土复合胶凝材料的制备及水化机理[J]. 硅酸盐通报, 2022, 41(5): 1724-1733.
	YUAN Zhengping, GENG Xinyang, WANG Fulin. Preparation and hydration mechanism of alkali-activated lead smelting slag-metakaolin composite cementitious materials[J]. Bulletin of the Chinese Ceramic Society, 2022, 41(5): 1724-1733.
12	YLINIEMI Juho, PESONEN Janne, TIAINEN Minna, et al. Alkali activation of recovered fuel-biofuel fly ash from fluidised-bed combustion: Stabilisation/solidification of heavy metals[J]. Waste Management, 2015, 43: 273-282.
13	VANDEVENNE Niels, IACOBESCU Remus Ion, CARLEER Robert, et al. Alkali-activated materials for radionuclide immobilisation and the effect of precursor composition on Cs/Sr retention[J]. Journal of Nuclear Materials, 2018, 510: 575-584.
14	HU Xiang, SHI Caijun, SHI Zhenguo, et al. Compressive strength, pore structure and chloride transport properties of alkali-activated slag/fly ash mortars[J]. Cement and Concrete Composites, 2019, 104: 103392.
15	李爽, 刘青科, 肖啸, 等. 碱激发矿渣/偏高岭土复合材自收缩特性研究[J]. 非金属矿, 2023, 46(1): 91-94.
	LI Shuang, LIU Qingke, XIAO Xiao, et al. Study on the autogenous shrinkage of metakaolin modified alkali-activated slag cement[J]. Non-Metallic Mines, 2023, 46(1): 91-94.
16	WANG J N, YU R, XU W Y, et al. A novel design of low carbon footprint ultra-high performance concrete (UHPC) based on full scale recycling of gold tailings[J]. Construction and Building Materials, 2021, 304: 124664.
17	王大鹏, 吴凯. 碱激发矿渣-金尾矿基泡沫混凝土的制备及其特性研究[J]. 矿业研究与开发, 2023, 43(5): 216-222.
	WANG Dapeng, WU Kai. Study on preparation and properties of alkali activated slag-gold tailings based foam concrete[J]. Mining Research and Development, 2023, 43(5): 216-222.
18	TANTAWY M A, AHMED Salwa A, ABDALLA Elham M, et al. Immobilization of copper ions laden Kaolin waste: Influence of thermal treatment on its immobilization in cement paste[J]. Journal of Material Cycles and Waste Management, 2016, 18(2): 263-272.
19	GUO Xueyi, QIN Hong, TIAN Qinghua, et al. The efficacy of a new iodination roasting technology to recover gold and silver from refractory gold tailing[J]. Journal of Cleaner Production, 2020, 261: 121147.
20	吴燕开, 胡晓士, 胡锐, 等. 烧碱激发钢渣粉在淤泥质土中的试验研究[J]. 岩土工程学报, 2017, 39(12): 2187-2194.
	WU Yankai, HU Xiaoshi, HU Rui, et al. Experimental study on caustic soda-activated steel slag powder in muddy soil[J]. Chinese Journal of Geotechnical Engineering, 2017, 39(12): 2187-2194.
21	王东星, 王宏伟, 邹维列, 等. 碱激发粉煤灰固化淤泥微观机制研究[J]. 岩石力学与工程学报, 2019, 38(S1): 3197-3205.
	WANG Dongxing, WANG Hongwei, ZOU Weilie, et al. Study on microscopic mechanism of solidification of sludge by alkali-activated fly ash[J]. Chinese Journal of Rock Mechanics and Engineering, 2019, 38(S1): 3197-3205.
22	AMER Ismail, KOHAIL Mohamed, EL-FEKY M S, et al. A review on alkali-activated slag concrete[J]. Ain Shams Engineering Journal, 2021, 12(2): 1475-1499.
23	DAI Xiaodi, AYDIN Serdar, YARDIMCI Mert Yücel, et al. Effect of temperature on the fresh and hardened state properties of alkali-activated slag/fly ash mixtures[J]. Materials and Structures, 2023, 56(5): 107.
24	迟凤霞, 韩博, 程沁灵, 等. 激发剂内部参数对碱激发注浆材料性能的影响[J]. 硅酸盐通报, 2021, 40(5): 1751-1759.
	CHI Fengxia, HAN Bo, CHENG Qinling, et al. Effect of internal parameters of activator on performance of alkali-activated grouting material[J]. Bulletin of the Chinese Ceramic Society, 2021, 40(5): 1751-1759.
25	陈柯宇, 吴大志, 胡俊涛. 基于组分的地聚合物胶凝材料反应机理及其制备参数的研究进展[J]. 硅酸盐通报, 2020, 39(7): 2033-2041.
	CHEN Keyu, WU Dazhi, HU Juntao. Advances in the reaction mechanism and preparation parameters of geopolymer binder material based on components[J]. Bulletin of the Chinese Ceramic Society, 2020, 39(7): 2033-2041.
26	邓永锋, 吴子龙, 刘松玉, 等. 地聚合物对水泥固化土强度的影响及其机理分析[J]. 岩土工程学报, 2016, 38(3): 446-453.
	DENG Yongfeng, WU Zilong, LIU Songyu, et al. Influence of geopolymer on strength of cement-stabilized soils and its mechanism[J]. Chinese Journal of Geotechnical Engineering, 2016, 38(3): 446-453.
27	ZHOU Shukui, LI Jiali, RONG Lishan, et al. Immobilization of uranium soils with alkali-activated coal gangue-based geopolymer[J]. Journal of Radioanalytical and Nuclear Chemistry, 2021, 329(3): 1155-1166.
28	WANG Fulin, CHEN Guoliang, JI Lu, et al. Preparation and mechanical properties of cemented uranium tailing backfill based on alkali-activated slag[J]. Advances in Materials Science and Engineering, 2020, 2020: 6345206.

[1]	何子晗, 李文譞, 李彦宇, 王雪超, 杨始蓉, 谢慧娜, 李杰. 水环境中抗生素抗性基因研究进展[J]. 化工进展, 2024, 43(S1): 533-544.
[2]	郝康安, 周颖, 刘川, 俞润昊, 黄安荣, 吴翀, 左晓玲. 荧光水凝胶基信息储存材料的构筑及其加密性能研究进展[J]. 化工进展, 2024, 43(9): 5013-5025.
[3]	赵星程, 贾方旭, 刘晨雨, 韩宝红, 梅宁, 姚宏. 实际规模PN/A工艺载体挂膜性能与微生物群落[J]. 化工进展, 2024, 43(9): 5242-5249.
[4]	刘芳, 刘海霞, 魏云霞, 马明广. 凹凸棒/琼脂复合气凝胶的制备及太阳能界面蒸发性能[J]. 化工进展, 2024, 43(9): 5329-5338.
[5]	孙燕, 谢晓阳, 冯倩颖, 郑璐, 何皎洁, 杨利伟, 白波. 基于单宁酸-铁(Ⅲ)改性正渗透膜制备及抗污染性能[J]. 化工进展, 2024, 43(9): 5309-5319.
[6]	王洋, 张苗苗, 吕阳, 侯翠红, 危常州, 马文奇, 张福锁, 申建波. pH响应材料及其在智能肥料中的应用[J]. 化工进展, 2024, 43(8): 4477-4489.
[7]	郑云香, 高艺伦, 李宴汝, 刘青霖, 张浩腾, 王向鹏. 氨基三乙酸酐改性多孔双网络水凝胶的制备及吸附性能[J]. 化工进展, 2024, 43(8): 4542-4549.
[8]	张蕾, 杜红英, 冯文浩, 郭军康. 基于二维光热材料的界面太阳能光热蒸发系统优化[J]. 化工进展, 2024, 43(8): 4571-4586.
[9]	武哲, 曲树光, 冯练享, 曾湘楚. 海藻酸钠/微晶纤维素复合水凝胶对水中甲基橙和亚甲基蓝的吸附性能与机理[J]. 化工进展, 2024, 43(8): 4681-4693.
[10]	胡锐, 李先如, 朴玮玲, 冯盼, 罗磊, 罗刚, 卫皇曌, 刘振刚, 张士成. 有机废物水热转化设备与技术研究进展[J]. 化工进展, 2024, 43(7): 3672-3691.
[11]	于立爽, 李青云, 刘兆明, 张淑茹, 刘幽燕, 唐爱星. 油菜花粉生物炭固定化脂肪酶催化蒎烯环氧化[J]. 化工进展, 2024, 43(7): 3996-4004.
[12]	何弈雪, 秦先超, 马伟芳. 过硫酸盐高级氧化原位修复地下水中卤代烃污染研究进展[J]. 化工进展, 2024, 43(7): 4072-4088.
[13]	刘世达, 侯栓弟, 刘忠生. 中美石化行业源空气污染物控制标准对比分析与展望和建议[J]. 化工进展, 2024, 43(7): 4089-4101.
[14]	杨昕, 钟承韡, 杨志山, 朱韦韦, 王文浩, 余江. 人工仿真菱铁矿及其衍生材料催化修复PAHs污染土壤[J]. 化工进展, 2024, 43(7): 4118-4127.
[15]	罗臻, 王庆吉, 王占生, 杨雪莹, 谢加才, 王浩. 炼化污染场地抽出水强氧化短程处理工艺[J]. 化工进展, 2024, 43(7): 4155-4163.

Ca(OH)₂注浆对碱激发固化铀尾矿渣性能的影响

Effect of Ca(OH)₂ grouting on the property of alkali-activated solidified uranium tailing slags

RichHTML

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

图/表 18

参考文献 28

相关文章 15

编辑推荐

Metrics

本文评价