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-

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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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