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

doi:10.15541/jim20190397

Abstract

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

CLC Number:

TQ174

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.

Figures/Tables 7

Fig. 1 Synthetic route for AO-HTC

Fig. 2 Design of experimental apparatus

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-

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

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-

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

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

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