An activated calcite-loaded hydroxyapatite PRB media for uranium ion removal from aqueous solution

doi:10.13745/j.esf.sf.2021.2.21

Abstract

Abstract:

Through static and dynamic tests, this paper investigated the removal efficiency and mechanism of uranium ion adsorption by calcite-loaded hydroxyapatite composites (CLHC) that was synthesized by the sol-gel method. The experimental results show that the CLHC surface was covered by hydroxyapatite after synthesis and had a strong affinity for uranium ions. The removal rate could reach 100% under the conditions of additive concentration of 0.5 g/L, solution pH of 4, initial uranium concentration of 5.0 mg/L, and experimental period of 2 hours. The adsorption processes of uranium can be described by a langmuir isotherm adsorption model, an intraparticle diffusion-adsorption dynamics model, or a quasi secondary adsorption kinetics model. CLHC has better adsorption ability and longer service life than quartz sand-loaded hydroxyapatite. Uranium ions were always hexavalent during adsorption, mainly by means of chemical adsorption via ion exchange. The results of this study provide a theoretical basis for the application of permeable reactive wall to groundwater remediation.

Key words: PRB, hydroxyapatite, aquifer, calcite, uranium ion

CLC Number:

X523

ZHANG Weimin, WANG Zhen, QIAN Cheng, GUO Yadan, LIU Haiyan. An activated calcite-loaded hydroxyapatite PRB media for uranium ion removal from aqueous solution[J]. Earth Science Frontiers, 2021, 28(5): 175-185.

Figures/Tables 18

Table 1 Experimental parameters for the static tests

试验条件	单位	取值	方法
CLHC用量	g·L^-1	0.3,0.5,0.7,0.9,1.0	25 ℃恒温气浴,167 r/min震荡,震荡时间为4 h,U初始浓度为5.0 mg·L^-1
溶液pH值		2.0,3.0,4.0,5.5,6.5,7.5
试验周期	min	10,30,60,90,120,180,240
U的初始浓度	mg·L^-1	2,5,7,9,11

Fig.1 Diagram of the dynamic column

Fig.2 Effect of dosage (a), pH value (b), experimental period (c), and U content (d) on U adsorption

Fig.3 Fitting results of (a) aquasi first order dynamic model (FODM) or (b) a quasi second order dynamic model (SODM)

Table 2 Characteristic fitting parameters using FODM and SODM

浓度	FODM参数				SODM参数
浓度	Q_e/ (mg·g^-1)	a₁/ min^-1	R²		Q_e/ (mg·g^-1)	a₂/ (g·mg^-1·min^-1)	R²
5 mg·L^-1	4.36	0.02	0.96		10.4	0.01	0.99

Fig.4 Fitting results of an intraparticle diffusion dynamics model (PDDM)

Table 3 Characteristic fitting parameters using LIAM and FIAM

温度	LIAM				FIAM
温度	q_m/ (mg·g^-1)	K_L/ (L·mg^-1)	R²		K_F/ (L·mg^-1)	1/n	R²
26 ℃	11.7	1.37	0.995		8.52	0.107	0.871

Fig.5 Fitting results with (a) the langmuir isothermal adsorption model (LIAM) or (b) the freundlich isothermal adsorption model (FIAM)

Fig.6 Breakthrough curves of Column A and B adsorbing U(Ⅵ)

Table 4 Statistical table of test parameters for dynamic columns A and B

编号	CLHC	U的初始浓度/ (mg·L^-1)	流量/ (L·h^-1)	pH值	穿透时间点	耗竭时间点	间隔/h
A	方解石	5.0	0.32	4.0	107 h时	624 h时	516
B	石英砂	5.0	0.32	4.0	101 h时	581 h时	482

Table 5 Parameters of Columns A and B

编号	U的初始浓度/ (mg·L^-1)	流速/ (L·h^-1)	总时间/ h	CLHC用量/g	柱吸附U的总量/g	柱饱和单位吸附量/ (mg·g^-1)	柱总流量/L	进液总U 量/g
A	5.0	0.32	627	29.8	0.42	14.3	197	0.99
B	5.0	0.32	557	29.1	0.36	12.5	183	0.91

Fig.7 Fitting results using the Thomas or Yoon-Nelson models for columns A and B

Fig.8 Results of scanning electron microscopy. (a) Calcite before adsorption; (b) CLHC before adsorption;(c) Calcite after adsorption; (b) CLHC after adsorption.

Fig.9 EDS spectra and scanning electron micrographs showing the sampling spots for calcite before (a, b) and after (c, d) adsorption

Fig.10 EDS spectra and scanning electron micrographs showing the sampling spots for CLHD before (a, b) and after (c, d) adsorption

Fig.11 X-ray diffraction pattern for CLHC

Fig.12 Broad (a) and narrow (b) band spectra of CLHC before and after tests

Fig.13 Uranium narrow band spectrum peak fitting

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