Efficient Adsorption of Radioactive Iodide by Copper/Palygorskite Composite

doi:10.15541/jim20200663

Abstract

Abstract:

To solve the disadvantages of low adsorption capacity, low utilization and easily desorption of traditional Cu-based adsorbents for radioactive iodide, the inevitable product of nuclear fission, Cu/Palygorskite composite (Cu@PAL) was synthesized through impregnation-reduction method, characterized and applied to remove I^- anions based on the excellent traits of PAL, such as cheap, abundant exchangeable cations and interstratified structure. Results indicate that there are about 7.5wt% copper nanoparticles loaded into PAL for the as-prepared composite. Cu@PAL has better performance in the adsorption of iodide as compared with traditional Cu-based adsorbents, with 72% utilization efficiency and excellent adsorption capacity of 116.1 mg/g. Cu@PAL is suitable for adsorption of I ^- anions under the conditions of neutral, weak acid and the coexistence of interference ions. In addition, the composite exhibit strong oxidation resistance, and the adsorbed product also has strong stability due to the copper stored in the PAL structure.

Key words: palygorskite, elemental copper, radioactive iodide, desorption efficiency, adsorption capacity

CLC Number:

TB333

YU Xiangkun, LIU Kun, LI Zhipeng, ZHAO Yulu, SHEN Jinyou, MAO Ping, SUN Aiwu, JIANG Jinlong. Efficient Adsorption of Radioactive Iodide by Copper/Palygorskite Composite[J]. Journal of Inorganic Materials, 2021, 36(8): 856-864.

Figures/Tables 18

Fig. 1 SEM images of the samples (a) PAL, (b) Cu 2+@PAL, (c) Cu@PAL and (d) EDX pattern of Cu@PAL

Table1 Chemical analysis (XRF) of PAL and Cu@PAL/wt%

Composition	PAL	Cu@PAL
SiO₂	60.96	59.87
MgO	9.36	8.12
Al₂O₃	12.20	11.07
Fe₂O₃	8.00	7.51
CaO	5.55	0.46
CuO	0.01	9.83
Na₂O	0.12	0.01
LOI	3.80	3.13

Fig. 2 (a) XRD patterns of the samples and (b) structural schematic diagram of Cu@PAL

Fig. 3 (a) TEM image of Cu2+@PAL and elemental mappings of (b) N, (c) O, (d) Al, (e) Si, and (f) Cu

Fig. 4 (a) TEM image of Cu@PAL and elemental mappings of (b) N, (c) O, (d) Al, (e) Si, and (f) Cu; and high magnification TEM (g) and HRTEM (h) images of Cu@PAL

Fig. 5 XPS spectra of the samples (a) Survey scans; (b) Cu2p core level spectra; (c) I 3d core level spectrum

Fig. 6 (a) TGA curves and (b) FT-IR spectra of the samples

Fig. 7 (a) N2 adsorption-desorption isotherms and (b) pore diameter distributions of the samples

Fig. 8 (a) Adsorption capacity of I- anions on Cu@PAL and (b) XRD patterns of adsorption products in the solution with different pH

Fig. 9 (a) Adsorption isotherm of the samples, fitting curves of (b) Langmuir model and (c) Frenudlich model for adsorption isotherm of Cu@PAL

Table 2 Comparison of several Cu based adsorbents for iodide adsorption

Adsorbent	pH	Q_e/ (mg∙g^-1)	Utilization efficiency/%	Ref.
Cuprite sulfide	7	6.1	—	[27]
Cu₂O/Cu-C	7	41.2	10.38	[28]
Hollow Cu/Cu₂O	7	33.0	1.85	[20]
Core-shell Cu/Cu₂O	7	22.9	1.4	[12]
Cu	7	6.35	0.32	[29]
Cu/PAL	7	116.1	71.98	This work

Table 3 Isotherm parameters for the adsorption of I- anions by Cu@PAL

Langmuir model			Frenudlich model
Q_m/(mg∙g^-1)	K_l	R²	K_f	1/n	R²
1.02915	0.86041	0.99632	0.38173	0.51042	0.81026

Table 4 Adsorption properties of Cu@PAL and nano Cu exposed to air

Time/h	Q_e/(mg∙g^-1)
Time/h	Cu@PAL	Nano-Cu
0	74.2	234.7
12	69.4	133.8
24	68.1	110.4
48	64.1	104.6
72	60.2	96.3
144	58.7	88.4

Fig. 10 SEM (a) and TEM (b) and HRTEM (c) images of I-Cu@PAL

Fig. 11 Absorption kinetic curve (a), fitting curves of the pseudo first order kinetic model (b) and pseudo second order kinetic model (c) for adsorption kinetic of Cu@PAL

Table 5 Kinetic parameters for the adsorption of I- by Cu@PAL

Pseudo-first-order			Pseudo-second-order
Q_m/ (mg∙g^-1)	k₁/(g∙(mmol∙ g^-1)^-1)	R²	Q_m/ (mg∙g^-1)	k₂/(g∙(mmol∙ g^-1)^-1)	R²
56.10	0.4469	0.9704	74.1840	0.03549	0.9976

Fig. 12 Effect of (a) anion and (b) cation on the adsorption of Cu@PAL

Table 6 Leaching or desorption efficiencies of Cu@PAL and nano-Cu after adsorption

Adsorbent	c_NaCl/(mol∙L^-1)	Desorption efficiency/%
Cu@PAL	0	21.3
Cu@PAL	0.1	32.1
Nano-Cu	0	87.4
Nano-Cu	0.1	94.1

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