沸石材料吸附水中放射性锶和铯的研究进展

doi:10.16085/j.issn.1000-6613.2018-1257

摘要/Abstract

摘要：

放射性锶和铯是核工业生产过程中重要的核裂变产物，也是放射性废水中含量较多的放射性污染物，具有较长的半衰期和持续的生物毒性。本文综述了近几年国内外采用天然沸石、合成沸石和复合沸石吸附去除水中放射性锶、铯的研究进展。重点阐述了海藻酸盐、聚丙烯腈、炭材料以及磁改性金属与沸石构成的复合吸附材料对水中放射性锶、铯的吸附。复合沸石可以解决沸石粒径小、难分离、稳定性差等难题，强化了沸石的实用性。从吸附平衡时间、最大吸附容量、酸碱耐受度等方面归纳了沸石材料对水中放射性锶、铯的吸附特性，并分析总结了三类沸石的优缺点。最后，针对沸石材料在处理放射性锶、铯废水中的应用，展望了未来的研究方向，指出可以在降低原水浓度、开发组合工艺和加强模型模拟等方面的研究进行完善，从而推动沸石材料未来在工程技术领域的应用。

关键词: 沸石, 放射性核素, 锶, 铯, 吸附

Abstract:

Radioactive strontium and cesium are the most important nuclear fission products in the process of nuclear industry and the most abundant radioactive pollutants in nuclear waste water. They have long half-life and persistent biological toxicity. This paper reviewed the latest advances at home and abroad in removing radioactive strontium and cesium from aqueous solutions by natural zeolites, synthetic zeolites and composite zeolites. It focused on the adsorption of radioactive cesium and strontium in aqueous solution by composite adsorbents, which are the compounding of alginate, polyacrylonitrile, carbon materials or magnetically modified metal on zeolites. The composite zeolites could solve the problems of small in particle size, difficult in separation, poor in stability, and enhance the applicability of the zeolite. The adsorption characteristics of zeolite materials on radioactive strontium and cesium in aqueous solution were summarized from the aspects of adsorption equilibrium time, maximum adsorption capacity and acid-base tolerance. The advantages and disadvantages of the three types of zeolites were analyzed and summarized. Furthermore, future research directions are prospected aiming at the application of zeolite materials in the treatment of radioactive cesium and strontium from aqueous solution. It is pointed out that the research on reducing raw water concentration, developing combined process and strengthening model simulation can promote the application of zeolite materials in engineering technology in future.

Key words: zeolite, radionuclides, strontium, cesium, adsorption

中图分类号:

X591

张振国, 张铭栋, 顾平, 张光辉. 沸石材料吸附水中放射性锶和铯的研究进展[J]. 化工进展, 2019, 38(04): 1984-1995.

Zhenguo ZHANG, Mingdong ZHANG, Ping GU, Guanghui ZHANG. Progress in adsorption of radioactive strontium and cesium from aqueous solution on zeolite materials[J]. Chemical Industry and Engineering Progress, 2019, 38(04): 1984-1995.

图/表 10

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沸石种类	主要实验条件	平衡时间/min	最大吸附容量^②/mg?g^-1	pH对吸附能力的影响	参考文献
塞尔维亚斜发沸石	C ₀=5～1000mg?L^-1， m/V=5g?L^-1， pH=5， 20℃	360	9.80	2~10时吸附稳定， >10时急剧增加	[30]
A型沸石	C ₀=100～1000mg?L^-1， m/V =1g?L^-1， pH=6， 25℃	90～120	303.00	<5时受到抑制， 6～8时最高	[42]
Na A-X型沸石	C ₀=100～1000mg?L^-1， m/V=1g?L^-1， pH=7， 25℃	90	312.50	2～6时不断增加， 6～9时趋于平稳	[48]
纳米Y型沸石	C ₀=50～1500mg?L^-1， m/V =2g?L^-1， 25℃	60^①	1342.34	—	[56]
MWCNT增强海藻酸钠A型沸石	C ₀=20～100mg?L^-1②， m/V =1.375g?L^-1， 25℃	700^①	107.50	—	[60]
PAN-沸石纳米复合材料	C ₀=43.81~4381mg?L^-1， m/V =10g?L^-1， 25℃	90	98.13	2～7时不断增加， >7时缓慢下降	[63]
炭/天然斜发沸石复合材料	C ₀=50～700mg?L^-1， m/V =2g?L^-1， pH=5.7， 25℃	180	95.62	2～10时不断增加	[66]
磁性斜发沸石	C ₀=50～400mg?L^-1， m/V =5g?L^-1， pH=4， 25℃	1200	20.58	2～10时不断增加， >10时急剧增加	[69]
磁性纳米A型沸石	C ₀=87.62～8762mg?L^-1， m/V =10g?L^-1， 25℃	60^①	89.05	3～7时不断增加， 7～9时趋于平稳	[71]
磁性纳米Y型沸石	C ₀=50～1000mg?L^-1， m/V =2g?L^-1， 25℃	120	228.63	4～8时不断增加	[73]

沸石种类	主要实验条件	平衡时间/min	最大吸附容量^②/mg?g^-1	pH对吸附能力的影响	参考文献
塞尔维亚斜发沸石	C ₀=5～1000mg?L^-1， m/V=5g?L^-1， pH=5， 20℃	360	9.80	2~10时吸附稳定， >10时急剧增加	[30]
A型沸石	C ₀=100～1000mg?L^-1， m/V =1g?L^-1， pH=6， 25℃	90～120	303.00	<5时受到抑制， 6～8时最高	[42]
Na A-X型沸石	C ₀=100～1000mg?L^-1， m/V=1g?L^-1， pH=7， 25℃	90	312.50	2～6时不断增加， 6～9时趋于平稳	[48]
纳米Y型沸石	C ₀=50～1500mg?L^-1， m/V =2g?L^-1， 25℃	60^①	1342.34	—	[56]
MWCNT增强海藻酸钠A型沸石	C ₀=20～100mg?L^-1②， m/V =1.375g?L^-1， 25℃	700^①	107.50	—	[60]
PAN-沸石纳米复合材料	C ₀=43.81~4381mg?L^-1， m/V =10g?L^-1， 25℃	90	98.13	2～7时不断增加， >7时缓慢下降	[63]
炭/天然斜发沸石复合材料	C ₀=50～700mg?L^-1， m/V =2g?L^-1， pH=5.7， 25℃	180	95.62	2～10时不断增加	[66]
磁性斜发沸石	C ₀=50～400mg?L^-1， m/V =5g?L^-1， pH=4， 25℃	1200	20.58	2～10时不断增加， >10时急剧增加	[69]
磁性纳米A型沸石	C ₀=87.62～8762mg?L^-1， m/V =10g?L^-1， 25℃	60^①	89.05	3～7时不断增加， 7～9时趋于平稳	[71]
磁性纳米Y型沸石	C ₀=50～1000mg?L^-1， m/V =2g?L^-1， 25℃	120	228.63	4～8时不断增加	[73]

沸石种类	主要实验条件	平衡时间 /min	最大吸附容量 /mg?g^-1	pH对吸附能力的影响	参考文献
塞尔维亚斜发沸石	C ₀=5～1000mg?L^-1， m/V =5g?L^-1， pH=5， 20℃	360	49.02^③	2～3时缓慢增加， 3～12时保持恒定	[30]
天然斜发沸石	C ₀=13.29g?L^-1， m/V=10g?L^-1， pH=5， 25℃ [K⁺]= 0.0119mol?L^-1	—	168.80^②	3～9时变化不大	[31]
天然菱沸石	C ₀=0～13290mg?L^-1， m/V=10g?L^-1， pH=5， 25℃， [K⁺]= 0.0119mol?L^-1	360	275.10^②	3～9时变化不大	[31]
天然丝光沸石	C ₀=0～13290mg?L^-1， m/V=10g?L^-1， pH=5， 25℃ [K⁺]= 0.0119mol?L^-1	360	256.50^②	3～9时变化不大	[31]
斜发沸石ZO	C ₀=7.9～3946.5mg?L^-1， m/V =10g?L^-1， pH=7， 30℃	60	236.31^③	3～9时影响不大	[32]
斜发沸石ZCh	C ₀=7.9～3946.5mg?L^-1， m/V =10g?L^-1， pH=7， 30℃	60	170.35^③	3～9时影响不大	[32]
A型沸石	C ₀=100～1000mg?L^-1， m/V=1g?L^-1， pH=6， 25℃	90～120	207.47^③	<5时受到抑制， 6～8时最高	[42]
Na A-X型沸石	C ₀=100～1000mg?L^-1， m/V =1g?L^-1， pH=7， 25℃	40^②	205.46^③	2～6时不断增加， 6～8时趋于平稳	[46]
纳米Y型沸石	C ₀=50～1500mg?L^-1， m/V =2g?L^-1， 25℃	60^②	893.09^③	—	[56]
MWCNT增强的海藻酸钠A型沸石	C ₀=50～250mg?L^-1②， m/V =1.375g?L^-1， 25℃	400^②	113.60^③	—	[60]
PAN-沸石纳米复合材料	C ₀=132.9～13290mg?L^-1， m/V =10g?L^-1， 25℃	90	214.10^③	2～7时不断增加， >7时缓慢下降	[63]
炭/天然斜发沸石复合材料	C ₀=400mg?L^-1， m/V =5g?L^-1， pH=5， 25℃	120	27.70^②	2～10时不断增加	[65]
磁性纳米A型沸石	C ₀=87.62～8762mg?L^-1， m/V =10g?L^-1， 25℃	80^②	229.30^③	3～7时不断增加， 7～9时趋于平稳	[71]
磁性纳米Y型沸石	C ₀=50～1000mg?L^-1， m/V =2g?L^-1， 25℃	120	298.50^③	4～6时不断增加， 6～8时缓慢下降	[73]

沸石种类	主要实验条件	平衡时间 /min	最大吸附容量 /mg?g^-1	pH对吸附能力的影响	参考文献
塞尔维亚斜发沸石	C ₀=5～1000mg?L^-1， m/V =5g?L^-1， pH=5， 20℃	360	49.02^③	2～3时缓慢增加， 3～12时保持恒定	[30]
天然斜发沸石	C ₀=13.29g?L^-1， m/V=10g?L^-1， pH=5， 25℃ [K⁺]= 0.0119mol?L^-1	—	168.80^②	3～9时变化不大	[31]
天然菱沸石	C ₀=0～13290mg?L^-1， m/V=10g?L^-1， pH=5， 25℃， [K⁺]= 0.0119mol?L^-1	360	275.10^②	3～9时变化不大	[31]
天然丝光沸石	C ₀=0～13290mg?L^-1， m/V=10g?L^-1， pH=5， 25℃ [K⁺]= 0.0119mol?L^-1	360	256.50^②	3～9时变化不大	[31]
斜发沸石ZO	C ₀=7.9～3946.5mg?L^-1， m/V =10g?L^-1， pH=7， 30℃	60	236.31^③	3～9时影响不大	[32]
斜发沸石ZCh	C ₀=7.9～3946.5mg?L^-1， m/V =10g?L^-1， pH=7， 30℃	60	170.35^③	3～9时影响不大	[32]
A型沸石	C ₀=100～1000mg?L^-1， m/V=1g?L^-1， pH=6， 25℃	90～120	207.47^③	<5时受到抑制， 6～8时最高	[42]
Na A-X型沸石	C ₀=100～1000mg?L^-1， m/V =1g?L^-1， pH=7， 25℃	40^②	205.46^③	2～6时不断增加， 6～8时趋于平稳	[46]
纳米Y型沸石	C ₀=50～1500mg?L^-1， m/V =2g?L^-1， 25℃	60^②	893.09^③	—	[56]
MWCNT增强的海藻酸钠A型沸石	C ₀=50～250mg?L^-1②， m/V =1.375g?L^-1， 25℃	400^②	113.60^③	—	[60]
PAN-沸石纳米复合材料	C ₀=132.9～13290mg?L^-1， m/V =10g?L^-1， 25℃	90	214.10^③	2～7时不断增加， >7时缓慢下降	[63]
炭/天然斜发沸石复合材料	C ₀=400mg?L^-1， m/V =5g?L^-1， pH=5， 25℃	120	27.70^②	2～10时不断增加	[65]
磁性纳米A型沸石	C ₀=87.62～8762mg?L^-1， m/V =10g?L^-1， 25℃	80^②	229.30^③	3～7时不断增加， 7～9时趋于平稳	[71]
磁性纳米Y型沸石	C ₀=50～1000mg?L^-1， m/V =2g?L^-1， 25℃	120	298.50^③	4～6时不断增加， 6～8时缓慢下降	[73]

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