偕胺肟水热碳对U(VI)-CO3/Ca-U(VI)-CO3的吸附性能研究

doi:10.15541/jim20190397

摘要/Abstract

摘要：

水热碳吸附材料具有制备工艺简单、合成条件温和、表面易改性等优点。本研究以可溶性淀粉为碳源, 在硝酸铈铵催化作用下, 将丙烯腈开环接枝到淀粉分子上, 通过水热反应和盐酸羟胺还原制备偕胺肟化水热碳(AO-HTC)。结合静态和动态吸附实验, 重点研究了溶液pH、碳酸根和钙离子浓度对AO-HTC吸附铀性能的影响, 通过Thomas和Yoon-Nelson模型探究AO-HTC吸附铀的动态过程。结果表明: 随着pH、碳酸根浓度和钙浓度的增加, AO-HTC吸附铀的容量逐渐降低; 掺杂5wt%AO-HTC土壤柱的穿透点和饱和点体积也随之减小。与纯土壤柱相比, 掺杂5wt%AO-HTC土壤柱的最大吸附容量(q_o)和吸附质穿透50%所需的时间(τ)增大了数倍。由此可见, AO-HTC是一种性能优异的可渗透性反应墙(PRB)介质, 有望用于修复铀污染土壤和地下水。

关键词: 偕胺肟基, 水热碳, U(VI)-CO₃/Ca-U(VI)-CO₃, 吸附

Abstract:

Hydrothermal carbon adsorption materials possess the advantages of simple preparation process, mild synthesis conditions and easy surface modification. In this UO₂ ²⁺speciation as a function of CO₃ ^2- concentration, soluble starch used as carbon source, acrylonitrile was grafted onto starch molecule through ring opening under the catalysis of cerium ammonium nitrate. Subsequently, amidoxime hydrothermal carbon spheres (AO-HTC) were successfully synthesized by hydrothermal reaction and hydroxylamine hydrochloride reduction. Meanwhile, static and dynamic adsorption experiments were performed to investigate the effects of solution pH, carbonate and calcium ion concentration on the adsorption performance of AO-HTC for uranium. And the dynamic adsorption process of AO-HTC for uranium was also studied by Yoon-Nelson and Thomas models. The results show that the adsorption capacity of AO-HTC, the volume of penetration point as well as saturation point in the penetration curve also decreases gradually with the increase of pH, carbonate concentration and calcium concentration. The maximum adsorption capacity (q_o) and the required time (τ) of adsorbate through 50% of 5% AO-HTC column are several times higher than that of pure soil column. Therefore, the research highlights that AO-HTC would act as an excellent permeable-reactive barriers (PRB) medium and expected to remediate uranium-contaminated soil and groundwater.

Key words: aminoxime, hydrothermal carbon, U(VI)-CO₃/Ca-U(VI)-CO₃, adsorption

中图分类号:

TQ174

张志宾, 周润泽, 董志敏, 曹小红, 刘云海. 偕胺肟水热碳对U(VI)-CO₃/Ca-U(VI)-CO₃的吸附性能研究[J]. 无机材料学报, 2020, 35(3): 352-358.

ZHANG Zhibin, ZHOU Runze, DONG Zhimin, CAO Xiaohong, LIU Yunhai. Adsorption of U(VI)-CO₃/Ca-U(VI)-CO₃ by Amidoxime-functionalized Hydrothermal Carbon[J]. Journal of Inorganic Materials, 2020, 35(3): 352-358.

图/表 7

图1 制备AO-HTC的路线图

Fig. 1 Synthetic route for AO-HTC

图2 动态吸附装置图

Fig. 2 Design of experimental apparatus

图3 pH(a)、CO32-浓度(b)、Ca2+浓度(c)对AO-HTC吸附铀容量的影响, pH(d)、CO32-浓度(e)、Ca2+浓度(f)对土壤柱和AO-HTC柱穿透曲线的影响

Fig. 3 Effects of pH (a) and CO32 (b) and Ca2+ concentration (c) on uranium adsorbed onto AO-HTC, breakthrough curves of soil column and AO-HTC column at different pH (d), CO32- (e) and Ca2+ concentration (f) (a) 1.0 mmol/L CO32-, 0.5 mmol/L Ca2+; (b) pH=6.0, 0.5 mmol/L Ca2+; (c) pH=6.0, 1.0 mmol/L CO32-; (d) 4.0 mmol/L CO32-, 2.0 mmol/L Ca2+; (e) pH=8.0, 2.0 mmol/L Ca2+; (f) pH=8.0, 4.0 mmol/L CO32-

图4 CO32-(a)和Ca2+浓度(b)对溶液中铀形态分布的影响

Fig. 4 U(VI) speciation as a function of CO32- concentration (a) and Ca2+ concentration (b) in water

图5 纯土柱(a, c, e)和 AO-HTC柱(b, d, f)在不同条件下的Thomas拟合直线

Fig. 5 Thomas kinetic plots for the adsorption of U(VI) on red soils (a, c, e) and AO-HTC columns (b, d, f) (a, b) Effect of pH; (c, d) Effect of carbonate; (e, f) Effect of calcium (a, b) 4.0 mmol/L CO32- , 2.0 mmol/L Ca2+; (c, d) pH=8.0, 2.0 mmol/L Ca2+; (e, f) pH=8.0, 4.0 mmol/L CO32-

表1 Thomas和Yoon-Nelson模型的拟合参数

Table 1 Parameters of Thomas and Yoon-Nelson models

	pH	CO₃^2- /(mmol·L^-1)	Ca²⁺ /(mmol·L^-1)	Thomas model			Yoon-Nelson model
	pH	CO₃^2- /(mmol·L^-1)	Ca²⁺ /(mmol·L^-1)	K_Th/(´10^-3, mL·min^-1·g^-1)	q_o/(´10^-2, mg∙g^-1)	R²	K_YN/min^-1	τ/min	R²
Soil column	7.0	4	2	2.089	1.5	0.93	0.043	76	0.93
	7.5			2.143	1.3	0.97	0.042	67	0.97
	8.0			2.161	1.1	0.96	0.043	55	0.96
AO-HTC column	7.0	4	2	0.338	8.8	0.91	0.014	444	0.91
	7.5			0.367	7.4	0.83	0.007	371	0.83
	8.0			0.683	5.3	0.91	0.014	266	0.81
Soil column	8.0	1	2	1.475	1.5	0.95	0.029	75	0.95
		2		1.797	1.1	0.96	0.036	55	0.96
		3		1.509	1.5	0.87	0.031	76	0.87
		4		2.161	1.1	0.96	0.043	55	0.96
AO-HTC column	8.0	1	2	0.364	9.8	0.95	0.007	492	0.95
		2		0.727	7.8	0.90	0.015	392	0.90
		3		0.619	6.1	0.92	0.012	307	0.92
		4		0.683	5.3	0.91	0.014	266	0.91
Soil column	8.0	4	0.5	1.367	1.8	0.96	0.027	94	0.96
			1.0	1.805	1.4	0.98	0.036	73	0.98
			1.5	2.275	1.0	0.95	0.046	52	0.95
			2.0	2.161	1.1	0.96	0.043	55	0.96
AO-HTC column	8.0	4	0.5	0.211	11.1	0.80	0.004	558	0.80
			1.0	0.239	7.8	0.94	0.005	393	0.94
			1.5	0.257	6.6	0.94	0.005	330	0.94
			2.0	0.683	5.3	0.91	0.014	266	0.91

图6 纯土柱(a, c, e)和AO-HTC柱(b, d, f)在不同条件下的Yoon-Nelson拟合直线

Fig. 6 Yoon-Nelson kinetic plots for the adsorption of U(VI) on red soils (a, c, e) and AO-HTC columns (b, d, f) (a,b) Effect of pH; (c, d) Effect of calcium; (e, f) Effect of carbonate (a, b) 4.0 mmol/L CO32-, 2.0 mmol/L Ca2+; (c, d) pH=8.0, 2.0 mmol/L Ca2+; (e, f) pH=8.0, 4.0 mmol/L CO32-

参考文献 38

[1]	ZHANG Z B, DONG Z M, WANG X X , et al. Ordered mesoporous polymer-carbon composites containing amidoxime groups for uranium removal from aqueous solutions. Chemical Engineering Journal, 2018,341:208-217.
[2]	ZENG J Y, ZHANG H, SUI Y , et al. New amidoxime-based material TMP-g-AO for uranium adsorption under seawater conditions. Industrial & Engineering Chemistry Research, 2017,56(17):5021-5032.
[3]	LIU Y, CAO X, HUA R , et al. Selective adsorption of uranyl ion on ion-imprinted chitosan/PVA cross-linked hydrogel. Hydrometallurgy, 2010,104(2):150-155.
[4]	ZHANG Z, ZHANG H, QIU Y , et al. Study on adsorption of uranium by phosphorylated graphene oxide. Sci. Sin. Chim., 2018,48:1-12.
[5]	MAYES R T, GORKA J, DAI S . Impact of pore size on the sorption of uranyl under seawater conditions. Industrial & Engineering Chemistry Research, 2016,55(15):4339-4343.
[6]	LI J, WANG X, ZHAO G , et al. Metal-organic framework-based materials: superior adsorbents for the capture of toxic and radioactive metal ions. Chem. Soc. Rev., 2018,47(7):2322-2356.
[7]	EBBS. Role of uranium speciation in the uptake and translocation of uranium by plants. Journal of Experimental Botany, 1998,49(324):1183-1190.
[8]	YAO Z . Review on remediation technologies of soil contaminated by heavy metals. Procedia Environmental Sciences, 2012,16(4):722-731.
[9]	LANDSBERGER S, TAMALIS D . Leaching dynamics of uranium in a contaminated soil site. Journal of Radioanalytical & Nuclear Chemistry, 2013,296(1):319-341.
[10]	DING D X, LI S M, HU N , et al. Bioreduction of U(VI) in groundwater under anoxic conditions from a decommissioned in situ leaching uranium mine. Bioprocess & Biosystems Engineering, 2015,38(4):661-670.
[11]	OBIRI-NYARKO F, GRAJALES-MESA S J, MALINA G . An overview of permeable reactive barriers for in situ sustainable groundwater remediation. Chemosphere, 2014,111:243-259.
[12]	RICHARDSON J P, NICKLOW J W . In situ permeable reactive barriers for groundwater contamination. Soil & Sediment Contamination, 2002,11(2):241-268.
[13]	KORNILOVYCH B, WIREMAN M, UBALDINI S , et al. Uranium removal from groundwater by permeable reactive barrier with zero-valent iron and organic carbon mixtures: laboratory and field studies. Metals, 2018,8(6):408-419
[14]	ZHANG W, GUO Y, PAN Z , et al. Remediation of uranium- contaminated groundwater using the permeable reactive barrier thchnique coupled with hydroxyapatite-coated quartz sands. Fresenius Environmental Bulletin, 2018,27(5):2703-2716.
[15]	LI Z J, WANG L, YUAN L Y , et al. Efficient removal of uranium from aqueous solution by zero-valent iron nanoparticle and its graphene composite. Journal of Hazardous Materials, 2015,290:26-33.
[16]	ZHANG Z, LIU J, CAO X , et al. Comparison of U(VI) adsorption onto nanoscale zero-valent iron and red soil in the presence of U(VI)-CO₃/Ca-U(VI)-CO₃ complexes. Journal of Hazardous Materials, 2015,300:633-642.
[17]	WILTAFSKY M K, SCHMIDTLEIN B, ROTH F X . Estimates of the optimum dietary ratio of standardized ileal digestible valine to lysine for eight to twenty-five kilograms of body weight pigs. Journal of Animal Science, 2009,87(8):2544-2553.
[18]	LIU X, WU J, ZHANG S , et al. Amidoxime-functionalized hollow carbon spheres for efficient removal of uranium from wastewater. ACS Sustainable Chemistry & Engineering, 2019,7(12):10800-10807.
[19]	LADSHAW A P, DAS S, LIAO W P , et al. Experiments and modeling of uranium uptake by amidoxime-based adsorbent in the presence of other ions in simulated seawater. Industrial & Engineering Chemistry Research, 2016,55(15):4241-4248.
[20]	PANG H B, KUO L J, WAI C M , et al. Elution of uranium and transition metals from amidoxime-based polymer adsorbents for sequestering uranium from seawater. Industrial & Engineering Chemistry Research, 2016,55(15):4313-4320.
[21]	HAN B, ZHANG E, CHENG G , et al. Hydrothermal carbon superstructures enriched with carboxyl groups for highly efficient uranium removal. Chemical Engineering Journal, 2018,338:734-744.
[22]	ZHANG Z B, DONG Z M, DAI Y , et al. Amidoxime-functionalized hydrothermal carbon materials for uranium removal from aqueous solution. RSC Advances, 2016,6(104):102462-102471.
[23]	YABUSAKI S B, FANG Y, LONG P E , et al. Uranium removal from groundwater via in situ biostimulation: field-scale modeling of transport and biological processes. J. Contam. Hydrol., 2007,93(1-4):216-235.
[24]	OMIDI M H, AZAD F N, GHAEDI M , et al. Synthesis and characterization of Au-NPs supported on carbon nanotubes: application for the ultrasound assisted removal of radioactive UO₂ ²⁺ ions following complexation with Arsenazo III: spectrophotometric detection, optimization, isotherm and kinetic study. J. Colloid. Interface Sci., 2017,504:68-77.
[25]	ZHANG Z B, LIU Y H, CAO X H , et al. Sorption study of uranium on carbon spheres hydrothermal synthesized with glucose from aqueous solution. Journal of Radioanalytical and Nuclear Chemistry, 2013,295(3):1775-1782.
[26]	HUANG F, XU Y, LIAO S , et al. Preparation of amidoxime polyacrylonitrile chelating nanofibers and their application for adsorption of metal ions. Materials, 2013,6(3):969-980.
[27]	ZHAO Y, LI J, ZHAO L , et al. Synthesis of amidoxime-functionalized Fe₃O₄@SiO₂ core-shell magnetic microspheres for highly efficient sorption of U(VI). Chemical Engineering Journal, 2014,235:275-283.
[28]	ZHANG Z B, LIU J, CAO X H , et al. Comparison of U(VI) adsorption onto nanoscale zero-valent iron and red soil in the presence of U(VI)-CO₃/Ca-U(VI)-CO₃ complexes. Journal of Hazardous Materials, 2015,300:633-642.
[29]	LIU J, ZHAO C, YUAN G , et al. Adsorption of U(VI) on a chitosan/ polyaniline composite in the presence of Ca/Mg-U(VI)-CO₃ complexes. Hydrometallurgy, 2018,175:300-311.
[30]	LI X, ZHANG M, LIU Y , et al. Removal of U(VI) in aqueous solution by nanoscale zero-valent iron(nZVI). Water Quality Exposure & Health, 2013,5(1):31-40.
[31]	CERRATO J M, BARROWS C J, BLUE L Y , et al. Effect of Ca²⁺ and Zn²⁺ on UO₂ dissolution rates. Environ. Sci. Technol., 2012,46(5):2731-2737.
[32]	KENNEDY D W, FREDRICKSON J K, BROOKS S C , et al. Inhibition of bacterial U(VI) reduction by calcium. Abstracts of the General Meeting of the American Society for Microbiology, 2003,37(9):1850-1858.
[33]	EL HAYEK E, TORRES C, RODRIGUEZ-FREIRE L , et al. Effect of calcium on the bioavailability of dissolved uranium(VI) in plant roots under circumneutral pH. Environ. Sci. Technol., 2018,52(22):13089-13098.
[34]	CHEN L F, YIN X B, YU Q , et al. Rapid and selective capture of perrhenate anion from simulated groundwater by a mesoporous silica-supported anion exchanger. Microporous Mesoporous Mat., 2019,274:155-162.
[35]	WANG X X, CHEN L, WANG L , et al. Synthesis of novel nanomaterials and their application in efficient removal of radionuclides. Sci. China-Chem., 2019,62(8):933-967.
[36]	MAHMOUD M A . Adsorption of U(VI) ions from aqueous solution using silicon dioxide nanopowder. Journal of Saudi Chemical Society, 2018,22(2):229-238.
[37]	YAKOUT S M, METWALLY S S, EL-ZAKLA T . Uranium sorption onto activated carbon prepared from rice straw: competition with humic acids. Applied Surface Science, 2013,280(8):745-750.
[38]	ZHANG Z B, DONG Z M, WANG X X , et al. Synthesis of ultralight phosphorylated carbon aerogel for efficient removal of U(VI): batch and fixed-bed column studies. Chemical Engineering Journal, 2019,370:1376-1387.

偕胺肟水热碳对U(VI)-CO₃/Ca-U(VI)-CO₃的吸附性能研究

Adsorption of U(VI)-CO₃/Ca-U(VI)-CO₃ by Amidoxime-functionalized Hydrothermal Carbon

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