The adsorption of U(VI) on chlorite: batch, modeling and XPS study

Qiang Jin; Yuxiong Wang; Xin Zhao; Ye Fan; Xinya Diao; Zongyuan Chen; Zhijun Guo

doi:10.1515/ract-2024-0278

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The adsorption of U(VI) on chlorite: batch, modeling and XPS study

Qiang Jin , Yuxiong Wang , Xin Zhao , Ye Fan , Xinya Diao , Zongyuan Chen und Zhijun Guo

Veröffentlicht/Copyright: 10. Mai 2024

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Aus der Zeitschrift Radiochimica Acta Band 112 Heft 6

Abstract

A mechanistic modelling of the adsorption processes onto individual minerals presenting in the near- and far-fields can greatly enhance the credibility of long-term safety assessments of granite-based geological repositories. In this study, the titration and U(VI) adsorption characteristics of chlorite, one of the major minerals of rock fractures, have been studied. Potentiometric titration curves at two ionic strengths (0.1 and 0.4 mol/L NaCl) are successfully interpreted by considering protonation/deprotonation reactions on generic edge sites (≡SOH) in the framework of a non-electrostatic surface complexation model (SCM). The adsorption of U(VI) on chlorite was reached after 24 h, the adsorption kinetics can be described by a pseudo-second-order model. A non-electrostatic SCM with three surface complexes (≡SOUO₂⁺, ≡SO(UO₂)₃(OH)₅ and ≡SO(UO₂)₃(OH)₇²⁻) was set up based on pH edges of U(VI) at adsorption equilibrium in the absence of CO₂. Additional, experimental data measured as a function of U(VI) concentration, solid-to-liquid ratio and carbonate concentration were well reproduced by the proposed model. Finally, parallel experiments were conducted using X-ray photoelectron spectroscopy (XPS) to analyze the variation of U(VI) surface species speciation at different pH values. The good agreement between SCM prediction and XPS analysis demonstrates the reliability of the model in predicting and quantifying the radionuclides retention by chlorite.

Keywords: U(VI); chlorite; adsorption; modeling; non-electrostatic model; XPS

Corresponding author: Qiang Jin and Zhijun Guo, MOE Frontiers Science Center for Rare Isotopes, Lanzhou University, 730000 Lanzhou, China; and Radiochemistry Laboratory, School of Nuclear Science and Technology, Lanzhou University, 730000 Lanzhou, China, E-mail: jinq@lzu.edu.cn (Q. Jin), guozhj@lzu.edu.cn (Z. Guo)

Funding source: National Natural Science Foundation of China

Award Identifier / Grant number: 12175094, 22176079

Funding source: Natural Science Foundation of Gansu Province, China

Award Identifier / Grant number: 22JR5RA480

Funding source: Fundamental Research Funds for the Central Universities

Award Identifier / Grant number: lzujbky–2022–sp05, lzujbky–2023–stlt01

Research ethics: Not applicable.
Author contributions: The authors have accepted responsibility for the entire content of this manuscript and approved its submission.
Competing interests: The authors state no conflict of interest.
Research funding: This work funded by the National Natural Science Foundation of China (Grant Nos. 12175094, 22176079), the Natural Science Foundation of Gansu Province, China (No. 22JR5RA480) and the Fundamental Research Funds for the Central Universities (lzujbky–2022–sp05, lzujbky–2023–stlt01).
Data availability: The raw data can be obtained on request from the corresponding author.

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Received: 2024-01-18

Accepted: 2024-04-01

Published Online: 2024-05-10

Published in Print: 2024-06-25

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https://doi.org/10.1515/ract-2024-0278

Schlagwörter für diesen Artikel

U(VI); chlorite; adsorption; modeling; non-electrostatic model; XPS