生物质基铀吸附材料的研究进展

doi:10.11949/0438-1157.20200921

摘要/Abstract

摘要：

铀资源是国家核工业发展的重要战略资源，安全可持续铀资源供应是核电健康发展的关键。除铀矿资源外，绿色海水提铀技术是最有应用潜力的铀资源供应途径。吸附法是海水提铀和含铀废水处理的常见方法，面对复杂的海洋环境，设计和制备吸附量大、选择性高的吸附材料成为解决问题的关键，以高附加值的生物质基材料为铀吸附剂是一种新型的可持续发展策略。本文详细综述了生物质基铀吸附材料的分类、制备方法及其吸附性能，概括了生物质基吸附材料的研究现状和热点，基于研究现状，展望了未来高效生物质基吸附材料在海水提铀方面的发展方向和研究趋势。

关键词: 吸附, 生物质基材料, 提取, 海水提铀, 含铀废水处理

Abstract:

Uranium resources are an important strategic resource for the development of the country's nuclear industry, and safe and sustainable uranium resource supply is the key to the healthy development of nuclear power. Except uranium ore resource, uranium extraction from seawater becomes the most potential way to provide uranium resource. Adsorption is a common method for uranium extraction from seawater and uranium-containing wastewater treatment. Facing the complex marine environment, the design and preparation of adsorbent materials with high efficiency and high selectivity is essential. It is a new sustainable development strategy to prepare high value-added biomass-based materials for uranium adsorption. The classification, preparation methods and adsorption properties of biomass-based adsorption materials were reviewed, the research status and hotspots of biomass-based adsorption materials are summarized. At the same time, the development direction and research trend of high-efficiency biomass-based adsorption materials in the future are forecasted.

Key words: adsorption, biomass-based material, extraction, uranium extraction from seawater, uranium-containing wastewater treatment

中图分类号:

王莹, 李倩, 曹丽霞, 李艳香, 李望良. 生物质基铀吸附材料的研究进展[J]. 化工学报, 2021, 72(3): 1205-1216.

WANG Ying, LI Qian, CAO Lixia, LI Yanxiang, LI Wangliang. Progress of biomass-based materials for uranium adsorption[J]. CIESC Journal, 2021, 72(3): 1205-1216.

图/表 6

图1 壳聚糖纤维的表面胺肟改性合成方案[22]

Fig.1 The synthesis of amidoxime modified chitosan fibers[22]

图2 (a) 新型磷酸化氧化石墨烯/壳聚糖复合材料GO、GO-CS 和GO-CS-P对铀的吸附行为随时间的变化；(b) 新型磷酸化氧化石墨烯/壳聚糖复合材料GO、GO-CS 和GO-CS-P中，溶液的pH对铀去除率的影响；(c) 铀溶液中U(Ⅵ) 形态随pH的变化分布；(d) 吸附等温线，用Langmuir 和Freundlich模型拟合的新型磷酸化氧化石墨烯/壳聚糖复合材料GO、GO-CS 和GO-CS-P 的吸附曲线[29]

Fig.2 (a) Time-dependent sorption behaviors of U(Ⅵ) on GO, GO-CS and GO-CS-P; (b) Effect of solution pH on the removal of U(Ⅵ) by GO, GO-CS and GO-CS-P; (c) pH-depended speciation of U(Ⅵ) in solution; (d) Sorption isotherm, Langmuir and Freundlich model fits of U(Ⅵ) on GO, GO-CS and GO-CS-P[29]

表1 壳聚糖基-铀吸附材料铀吸附性能对比

Table 1 Summarizes of chitosan-based materials and uranium adsorption abilities

类别	吸附剂名称	吸附条件	最高吸附量/(mg·g^-1)	文献
壳聚糖颗粒	戊二醛和硫脲交联磁性壳聚糖（TTG-MCTS）	C₀ = 40 ~ 140 mg·L^-1 pH = 5.00，0.60 g·L^-1	161.3	[18]
	二乙烯三胺五乙酸功能化磁性壳聚糖（DTPA-MCS）	C₀ = 10 ~ 100 mg·L^-1 pH = 5.00，0.40 g·L^-1	178.20	[19]
	三聚磷酸钠交联磁性壳聚糖树脂（TPP-MCR）	C₀ = 40 ~ 150 mg·L^-1 pH = 3.00，0.40 g·L^-1	166.70	[20]
	离子印迹磁性壳聚糖微球（IMCR）	C₀ = 15 ~ 420 mg·L^-1 pH = 5.00，1.00 g·L^-1	187.26	[21]
壳聚糖纤维	共混纤维吸附剂（PVP/CS fibers）	C₀ = 1~ 270 mg·L^-1 pH = 6.00，1.00 g·L^-1	167±25	[24]
壳聚糖纤维	壳聚糖纤维膜（CS-80%）	C₀ = 10 ~ 100 mg·L^-1 pH = 5.00，0.50 g·L^-1	196.74	[25]
壳聚糖复合材料	壳聚糖/氧化石墨烯复合材料（CS/GO）	C₀ = 2 ~ 100 mg·L^-1 pH = 5.00，0.15 g·L^-1	217.40	[27]
	多巴胺交联氧化石墨烯/壳聚糖气凝胶(GO@PDA/CS)	C₀ = 10 ~ 220 mg·L^-1 pH = 6.00，0.30 g·L^-1	415.90	[28]
	磷酸化的氧化石墨烯/壳聚糖复合材料（GO-CS-P）	C₀ = 2 ~ 140 mg·L^-1 pH = 5.00，0.05 g·L^-1	779.44	[29]
	磷酸化壳聚糖/羧甲基纤维素复合材料（CSP-CMCP）	C₀ = 10 ~ 120 mg·L^-1 pH = 5.00，0.05 g·L^-1	977.54	[30]
	壳聚糖-氧化石墨烯/ZIF泡沫吸附剂（GCZ8A）	C₀ = 2 ~ 120 mg·L^-1 pH = 8.00，0.20 g·L^-1	361.01	[31]

图3 胺肟改性纤维素材料 (a) 对铀的吸附量随pH的变化(C0 = 10 mg·L-1, V = 100 ml, sorbent dose (SD) = 0.03 g, time =8 h); (b) 对铀的吸附量随含铀溶液初始浓度的变化(V = 100 ml, SD = 0.03 g, pH = 5, time =8 h); (c) 吸附实验数据和吸附等温线的拟合曲线(V = 100 ml, SD = 0.03 g, pH = 5, time =8 h)；(d) 吸附实验数据和吸附动力学的拟合曲线(V = 100 ml, SD = 0.03 g, pH = 5) [50]

Fig.3 (a) The uranium adsorption capacity at different pH (C0 = 10 mg·L-1, V = 100 ml, sorbent dose (SD) = 0.03 g, time =8 h); (b) The uranium adsorption capacity at different initial concentration (V = 100 ml, SD = 0.03 g, pH = 5, time =8 h); (c) The experimental data and fitting curves of adsorption isotherms (V = 100 ml, SD = 0.03 g, pH = 5, time =8 h); (d) The experimental data and fitting curves of adsorption kinetics (V = 100 ml, SD = 0.03 g, pH = 5) (the counter ions of uranium were hydroxyl) [50]

表2 纤维素基-铀吸附材料海水提铀性能

Table 2 Summarizes of cellulose-based materials used for uranium extraction from seawater

吸附剂	吸附条件	最高吸附量/(mg·g^-1)	自然/模拟海水提铀	文献
丝瓜络 (LC-PAA-PEI)	C₀ = 50 ~ 350 mg·L^-1 pH = 6.00，0.40 g·L^-1	444.40	R>90%	[46]
大麻纤维 (HF-PE1-GDAC)	C₀ = 5 ~ 400 mg·L^-1 pH = 7.00，0.40 g·L^-1	414.93	R=71%	[48]
剑麻纤维 (ATMP-Sisal-150)	C₀ = 10 mg·L^-1 模拟海水	16	0.10 mg·g^-1 自然海水	[49]
纤维素纤维 (PAO-CFs)	C₀ = 2 ~ 18 mg·L^-1 pH = 5.00，0.30 g·L^-1	52.88	1.22 mg U·(g Ads)^-1	[50]

图4 超级铀酰结合蛋白纤维（SSUP）提取海水中的铀示意图[71]

Fig.4 Schematic diagram of uranium extraction from seawater by spidroin-based super uranyl-binding protein (SSUP) [71]

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