Optimizing iodine capture performance by metal–organic framework containing with bipyridine units

doi:10.1007/s11705-022-2218-3

Front. Chem. Sci. Eng.

2023, Vol. 17

Issue (4) : 395-403 https://doi.org/10.1007/s11705-022-2218-3

RESEARCH ARTICLE

Optimizing iodine capture performance by metal–organic framework containing with bipyridine units

Xinyi Yang^1,², Xiaolu Liu², Yanfang Liu², Xiao-Feng Wang¹(

), Zhongshan Chen², Xiangke Wang²(

)

¹. School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China
². College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, China

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Abstract

Radioactive iodine exhibits medical values in radiology, but its excessive emissions can cause environmental pollution. Thus, the capture of radioiodine poses significant engineering for the environment and medical radiology. The adsorptive capture of radioactive iodine by metal–organic frameworks (MOFs) has risen to prominence. In this work, a Th-based MOF (denoted as Th-BPYDC) was structurally designed and synthesized, consisting of [Th₆(μ₃-O)₄(μ₃-OH)₄(H₂O)₆]¹²⁺ clusters, abundant bipyridine units, and large cavities that allowed guest molecules diffusion and transmission. Th-BPYDC exhibited the uptake capacities of 2.23 g·g⁻¹ and 312.18 mg·g⁻¹ towards I₂ vapor and I₂ dissolved in cyclohexane, respectively, surpassing its corresponding analogue Th-UiO-67. The bipyridine units boosted the adsorption performance, and Th-BPYDC showed good reusability with high stability. Our work thus opened a new way for the synthesis of MOFs to capture radioactive iodine.

Keywords metal–organic framework iodine adsorption nuclear waste environmental remediation

Corresponding Author(s): Xiao-Feng Wang,Xiangke Wang

Online First Date: 15 December 2022 Issue Date: 24 March 2023

Cite this article:

Xinyi Yang,Xiaolu Liu,Yanfang Liu, et al. Optimizing iodine capture performance by metal–organic framework containing with bipyridine units[J]. Front. Chem. Sci. Eng., 2023, 17(4): 395-403.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-022-2218-3
https://academic.hep.com.cn/fcse/EN/Y2023/V17/I4/395

Fig.1 (a) View of the [Th₆(μ₃-O)₄(μ₃-OH)₄(H₂O)₆]¹²⁺ SBU, and the BPYDC ligand; (b) the tetrahedral cavity substructure in Th-BPYDC; (c) the octahedral cavity substructure in Th-BPYDC; (d) the 3D framework of Th-BPYDC; (e) displaying the 12-connected fcu topology of Th-BPYDC.

Fig.2 (a) XRD patterns of Th-BPYDC before and desolvated sample, together with calculated result; (b) XRD patterns of Th-UiO-67 and desolvated sample, together with calculated result; (c) TGA diagrams of Th-BPYDC and Th-UiO-67 after activation; (d) N₂ adsorption (filled symbols) and desorption (open symbols) isotherms measured at 77 K for Th-BPYDC and Th-UiO-67; SEM image of (e) Th-BPYDC and (f) Th-UiO-67.

Fig.3 (a) XRD patterns of Th-BPYDC after treatment in aqueous solution with pH from 1–10; (b) XRD patterns of Th-BPYDC after treatment in various organic solvents; (c) XRD patterns of Th-UiO-67 after treatment in aqueous solution with pH from 1–10; (d) XRD patterns of Th-UiO-67 after treatment in various organic solvents.

Fig.4 (a) Equilibrium adsorption isotherms for iodine adsorption on different MOF materials in cyclohexane solutions (iodine concentrations ranging from 50 to ~1200 ppm; fit lines for the Langmuir model are shown); (b) iodine adsorption kinetics on different MOF materials at an initial iodine concentration of ~200 ppm in cyclohexane solutions; (c) iodine vapor adsorption kinetics on different MOF materials at 75 °C; (d) recyclability of Th-BPYDC for iodine adsorption from cyclohexane solution.

Tab.1 Comparison of the performance of different adsorbents for iodine adsorption in cyclohexane

Fig.5 (a) XRD patterns of Th-BPYDC after iodine adsorption studies; (b) XRD patterns of Th-UiO-67 after iodine adsorption studies; FTIR spectra of (c) Th-BPYDC and (d) Th-UiO-67 before and after iodine adsorption studies; I_3d XPS spectra for (e) Th-BPYDC and (f) Th-UiO-67 after iodine adsorption studies.

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