Status and progress of research on uranium-containing wastewater treatment by phosphate mineral fixation

doi:10.19965/j.cnki.iwt.2023-0442

Abstract

Abstract:

The harmless and resourceful treatment of uranium-containing wastewater generated from uranium and uranium-polymetallic ore mining and metallurgy is a hot research topic in the field of nuclear resources and environment. This paper reviewed the current research status and progress of uranium phosphate mineral solidification method to treat uranium-containing wastewater. The solidification principles and effects of uranium solidification by soluble phosphate, uranium solidification by phosphorus-containing natural minerals,uranium solidification by synthetic phosphate adsorbent materials,and uranium solidification by bio-mediated organic phosphorus were introduced. Compared with other mineral uranium solidification processes,uranium solidification by phosphate minerals had the advantages of high efficiency,low cost and high product stability. The addition of metal cations in the process of phosphate uranium fixation determined the process of uranium fixation and the type of products. Among metal phosphate uranium fixation minerals,variable calcium uranium mica had the highest dissolution stability,which provided a new idea for the removal and recovery of uranium in low concentration uranium-containing solutions by phosphate mineral solidification.

Key words: uranium, uranium-containing wastewater, immobilization as minerals, uranium consolidation mechanism, mineralization

摘要：

铀矿及铀-多金属矿采冶过程产生的含铀废水的无害化与资源化是核资源与环境领域的研究热点。综述了磷酸盐矿物固铀法处理含铀废水的研究现状与进展，介绍了可溶磷酸盐固铀、含磷天然矿物固铀、人工合成磷酸盐吸附材料固铀、生物介导有机磷固铀的固化原理及效果。相较于其他矿物固铀工艺，磷酸盐矿物固铀具有效率高、成本低、产物稳定性强的优点。磷酸盐固铀过程中，金属阳离子种类决定着固铀成矿过程及产物种类，在众多金属磷酸盐固铀矿物中，变钙铀云母的溶解稳定性最高，这为磷酸盐矿物固铀法在低浓度含铀溶液中铀的脱除与回收提供了新的思路。

关键词: 铀, 含铀废水, 矿物固化法, 固铀机理, 矿化

CLC Number:

P579

Pingchao KE, Tingting ZHONG, Tiannan WU, Kunkun WANG, Jiale LI, Yipeng ZHOU, Zhanxue SUN. Status and progress of research on uranium-containing wastewater treatment by phosphate mineral fixation[J]. Industrial Water Treatment, 2024, 44(6): 34-39.

柯平超, 钟婷婷, 吴天楠, 王坤坤, 李家乐, 周义朋, 孙占学. 磷酸盐矿物固铀法处理含铀废水研究现状与进展[J]. 工业水处理, 2024, 44(6): 34-39.

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URL: https://www.iwt.cn/EN/10.19965/j.cnki.iwt.2023-0442

https://www.iwt.cn/EN/Y2024/V44/I6/34

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References 42

1	WINDE F， BRUGGE D， NIDECKER A，et al. Uranium from Africa：An overview on past and current mining activities—Re-appraising associated risks and chances in a global context［J］. Journal of African Earth Sciences，2017，129：759-778. doi:10.1016/j.jafrearsci.2016.12.004
2	LIU Bo， PENG Tongjiang， SUN Hongjuan，et al. Release behavior of uranium in uranium mill tailings under environmental conditions［J］. Journal of Environmental Radioactivity，2017，171：160-168. doi:10.1016/j.jenvrad.2017.02.016
3	何帆，罗威，王国辉，等. 稀土冶炼过程中铀、钍、镭等放射性核素的迁移［J］. 稀土，2018，39（5）：32-39.
	HE Fan， LUO Wei， WANG Guohui，et al. The migration of U，Th，Ra during the smelting of rare earth［J］. Chinese Rare Earths，2018，39（5）：32-39.
4	刘康，向秋林，师留印，等. 铀钼矿硫酸焙烧提取铀钼［J］. 中国有色金属学报，2019，29（4）：858-863.
	LIU Kang， XIANG Qiulin， SHI Liuyin，et al. U and Mo extraction from U-Mo ore during sulfuric acid roasting process［J］. The Chinese Journal of Nonferrous Metals，2019，29（4）：858-863.
5	SILVA R， COUTO D， TAVARES A，et al. Enhanced process route to remove fluorine and uranium from copper concentrades by selective sulfuric acid leaching［J］. Minerals Engineering，2021，170：107039. doi:10.1016/j.mineng.2021.107039
6	ZENG Sheng， SHEN Yuan， SUN Bing，et al. Fractal kinetic characteristics of uranium leaching from low permeability uranium-bearing sandstone［J］. Nuclear Engineering and Technology，2022，54（4）：1175-1184. doi:10.1016/j.net.2021.10.013
7	ZHOU Yipeng， LI Guangrong， XU Lingling，et al. Uranium recovery from sandstone-type uranium deposit by acid in situ leaching：An example from the Kujieertai［J］. Hydrometallurgy，2020，191：105209. doi:10.1016/j.hydromet.2019.105209
8	林莹，高柏，李元锋. 核工业低浓度含铀废水处理技术进展［J］. 山东化工，2009，38（3）：35-38. doi:10.3969/j.issn.1008-021X.2009.03.009
	LIN Ying， GAO Bai， LI Yuanfeng. Development of study on treatment technology for wastewater with low-level uranium content of nuclear industry［J］. Shandong Chemical Industry，2009，38（3）：35-38. doi:10.3969/j.issn.1008-021X.2009.03.009
9	IBRAHIM M E， ORABI A H， FALILA N I，et al. Processing of the mineralized Black Mica for the recovery of uranium，rare earth elements，niobium，and tantalum［J］. Hydrometallurgy，2020，197：105474. doi:10.1016/j.hydromet.2020.105474
10	GB/T 14848—2017 地下水质量标准［S］. doi:10.1109/ieeestd.2021.9491981
	GB/T 14848—2017 Standard for groundwater quality ［S］. doi:10.1109/ieeestd.2021.9491981
11	NOLAN J， WEBER K A. Natural uranium contamination in major U. S. aquifers linked to nitrate［J］. Environmental Science & Technology Letters，2015，2（8）：215-220. doi:10.1021/acs.estlett.5b00174
12	陈军强，曾威，王佳营，等. 全球和我国铀资源供需形势分析［J］. 华北地质，2021，44（2）：25-34.
	CHEN Junqiang， ZENG Wei， WANG Jiaying，et al. Analysis of supply and demand situation of uranium resources in the world and China［J］. North China Geology，2021，44（2）：25-34.
13	SINGH D K， HAREENDRAN K N，T S，et al. Development of a phosphate precipitation method for the recovery of uranium from lean tenor alkaline leach liquor［J］. Hydrometallurgy，2017，171：228-235. doi:10.1016/j.hydromet.2017.05.021
14	WEN Yongzhong， WEI Qiaosheng. Analysis on poisoning phenomenon of ion exchange resin and its solution［J］. Journal of Filtration & Separation，2014，24（4）：26-28.
15	DUFF M C， COUGHLIN J U， HUNTER D B. Uranium co-precipitation with iron oxide minerals［J］. Geochimica et Cosmochimica Acta，2002，66（20）：3533-3547. doi:10.1016/s0016-7037(02)00953-5
16	MCMASTER S A，RAM R， CHARALAMBOUS F，et al. Synthesis and characterisation of the uranium pyrochlore betafite〔（Ca，U）₂（Ti，Nb，Ta）₂O₇〕［J］. Journal of Hazardous Materials，2014，280：478-486. doi:10.1016/j.jhazmat.2014.07.062
17	NETTLETON K C A， NIKOLOSKI A N， COSTA M DA. The leaching of uranium from betafite［J］. Hydrometallurgy，2015，157：270-279. doi:10.1016/j.hydromet.2015.09.008
18	FRANKLAND V L， MILODOWSKI A E， READ D. Characterisation of meta-autunite：Towards identifying potential alteration products of spent nuclear fuel［J］. Applied Geochemistry，2020，123：104792. doi:10.1016/j.apgeochem.2020.104792
19	FOSTER R I， KIM K W， OH M K，et al. Effective removal of uranium via phosphate addition for the treatment of uranium laden process effluents［J］. Water Research，2019，158：82-93. doi:10.1016/j.watres.2019.04.021
20	GUDAVALLI R K. Effect of pH and temperature on the carbonate promoted dissolution of sodium meta-autunite［D］. Miami，USA：Florida International University，2012.
21	COURTOIS J， WANG Bin， ABONEE I N，et al. Bare and polyelectrolyte-coated calcium carbonate particles for seawater uranium extraction：An eco-friendly alternative［J］. Sustainable Energy & Fuels，2020，4（10）：5301-5312. doi:10.1039/d0se00785d
22	KORNILOVYCH B， KOVALCHUK I， TOBILKO V，et al. Uranium removal from groundwater and wastewater using clay-supported nanoscale zero-valent iron［J］. Metals，2020，10（11）：1421. doi:10.3390/met10111421
23	WELLMAN D M， PIERCE E M， VALENTA M M. Efficacy of soluble sodium tripolyphosphate amendments for the in situ immobilisation of uranium［J］. Environmental Chemistry，2007，4（5）：293. doi:10.1071/en07030
24	张晓峰，陈迪云，徐伟昌，等. 磷酸二氢钠去除铀的效果与机理［J］. 环境化学，2015，34（2）：321-326. doi:10.7524/j.issn.0254-6108.2015.02.2014050301
	ZHANG Xiaofeng， CHEN Diyun， XU Weichang，et al. Removal and mechanism of uranium by sodium dihydrogen phosphate［J］. Environmental Chemistry，2015，34（2）：321-326. doi:10.7524/j.issn.0254-6108.2015.02.2014050301
25	YU Zijing. Application study for metallogenic saleeite immobilization of uranium from wastewater［D］. Guangzhou：Guangzhou University，2022.
26	MEHTA V S， MAILLOT F， WANG Zheming，et al. Effect of reaction pathway on the extent and mechanism of uranium（Ⅵ） immobilization with calcium and phosphate［J］. Environmental Science & Technology，2016，50（6）：3128-3136. doi:10.1021/acs.est.5b06212
27	孔令军，俞紫荆，陈迪云，等. 一种含铀废水处理剂及处理含铀废水的方法：CN113461133A［P］. 2021-10-01.
28	SHI Qingpu， SU Minhua， YUVARAJA G，et al. Development of highly efficient bundle-like hydroxyapatite towards abatement of aqueous U（Ⅵ） ions：Mechanism and economic assessment［J］. Journal of Hazardous Materials，2020，394：122550. doi:10.1016/j.jhazmat.2020.122550
29	CHEN Baidi， WANG Jin， KONG Lingjun，et al. Adsorption of uranium from uranium mine contaminated water using phosphate rock apatite（PRA）：Isotherm，kinetic and characterization studies［J］. Colloids and Surfaces A：Physicochemical and Engineering Aspects，2017，520：612-621. doi:10.1016/j.colsurfa.2017.01.055
30	KRESTOU A， XENIDIS A， PANIAS D. Mechanism of aqueous uranium（Ⅵ） uptake by hydroxyapatite［J］. Minerals Engineering，2004，17（3）：373-381. doi:10.1016/j.mineng.2003.11.019
31	SHI Zhenqing， LIU Chongxuan， ZACHARA J M，et al. Inhibition effect of secondary phosphate mineral precipitation on uranium release from contaminated sediments［J］. Environmental Science & Technology，2009，43（21）：8344-8349. doi:10.1021/es9021359
32	LAMMERS L N， RASMUSSEN H， ADILMAN D，et al. Groundwater uranium stabilization by a metastable hydroxyapatite［J］. Applied Geochemistry，2017，84：105-113. doi:10.1016/j.apgeochem.2017.06.001
33	XIONG Xueying. Hydroxyapatite extracted from fishbone on uranium（Ⅵ） sorption from aqueous solution［D］. Guangzhou：Guangzhou University，2016.
34	HAN Meina， KONG Lingjun， HU Xingliang，et al. Phase migration and transformation of uranium in mineralized immobilization by wasted bio-hydroxyapatite［J］. Journal of Cleaner Production，2018，197：886-894. doi:10.1016/j.jclepro.2018.06.253
35	WANG Ting， QIAN Tianwei， HUO Lijuan，et al. Immobilization of hexavalent chromium in soil and groundwater using synthetic pyrite particles［J］. Environmental Pollution，2019，255：112992. doi:10.1016/j.envpol.2019.112992
36	MORRISON K D， ZAVARIN M， KERSTING A B，et al. Influence of uranium concentration and pH on U-phosphate biomineralization by Caulobacter OR37［J］. Environmental Science & Technology，2021，55（3）：1626-1636. doi:10.1021/acs.est.0c05437
37	李国武，邢晓琳，徐凯. 烧绿石及碱硬锰矿型矿物晶体化学及其核废料固化基材研究进展［J］. 中国材料进展，2016，35（7）：489-495. doi:10.7502/j.issn.1674-3962.2016.07.02
	LI Guowu， XING Xiaolin， XU Kai. The crystal structure and chemistry of pyrochlore- and hollandite-type minerals and their application as nuclear waste-forms［J］. Materials China，2016，35（7）：489-495. doi:10.7502/j.issn.1674-3962.2016.07.02
38	LAM S T， DOLAN K， LIU Wenguan，et al. Weak and strong hydrogen interactions on porous carbon materials in high-temperature systems ［J］. Journal of Nuclear Materials，2019，519：173-181. doi:10.1016/j.jnucmat.2019.03.036
39	SUN Jian， ZHOU Jing， HU Zhiwei，et al. Controllable sites and high-capacity immobilization of uranium in Nd₂Zr₂O₇ pyrochlore［J］. Journal of Synchrotron Radiation，2022，29（Pt 1）：37-44. doi:10.1107/s1600577521012558
40	WANG Lielin， LI Jiangbo， XIE Hua，et al. Solubility and ion-irradiation effects of uranium in Nd₂Zr₂O₇ pyrochlore［J］. Acta Physica Sinica，2018，67（19）：192801. doi:10.7498/aps.67.20181204
41	王赛男. 中性有氧环境中天然和合成黄铁矿氧化固铀的效率与机理研究［D］. 衡阳：南华大学，2021.
	WANG Sainan. Study on efficiency and mechanism of uranium fixation by natural and synthetic pyrite oxidation in neutral aerobic environment［D］. Hengyang：University of South China，2021.
42	WU Tiannan， WANG Mingbing， ZHONG Tingting，et al. Behavior of uranium immobilization with hydroxyapatite and dissolution stability of the immobilization product［J］. Journal of Radioanalytical and Nuclear Chemistry，2023，332（3）：647-657. doi:10.1007/s10967-023-08799-3

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