Fluoride ions adsorption from water by CaCO<sub>3</sub> enhanced Mn–Fe mixed metal oxides

doi:10.1007/s11705-022-2193-8

Front. Chem. Sci. Eng.

2023, Vol. 17

Issue (2) : 236-248 https://doi.org/10.1007/s11705-022-2193-8

RESEARCH ARTICLE

Fluoride ions adsorption from water by CaCO₃ enhanced Mn–Fe mixed metal oxides

Xinyuan Wang¹, Heriberto Pfeiffer², Jiangjiang Wei¹, Jinyu Wang¹(

), Jinli Zhang^1,³(

)

¹. School of Chemistry and Chemical Engineering/Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan, Shihezi University, Shihezi 832003, China
². Institute of Materials, National Autonomous University of Mexico, Mexico City 04510, Mexico
³. School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China

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Abstract

Novel CaCO₃-enhanced Mn–Fe mixed metal oxides (CMFC) were successfully prepared for the first time by a simple-green hydrothermal strategy without any surfactant or template combined with calcination process. These oxides were then employed as an adsorbent for adsorptive removal of excess fluoride ions. The adsorbent was characterized by SEM, XPS, XRD, FTIR, and BET analysis techniques. The adsorption property of CMFC toward fluoride ion was analyzed by batch experiments. In fact, CMFC exhibited adsorption capacity of 227.3 mg∙g^‒1 toward fluoride ion. Results showed that ion exchange, electrostatic attraction and chemical adsorption were the main mechanism for the adhesion of large amount of fluoride ion on the CMFC surface, and the high adsorption capacity responded to the low pH of the adsorption system. When the fluoride ion concentration was increased from 20 to 200 mg∙L^‒1, Langmuir model was more in line with experimental results. The change of fluoride ion adsorption with respect to time was accurately described by pseudo-second-order kinetics. After five cycles of use, the adsorbent still maintains a performance of 70.6% of efficiency, compared to the fresh adsorbent. Therefore, this material may act as a potential candidate for adsorbent with broad range of application prospects.

Keywords mesoporous materials metal oxides fluoride ion adsorption mechanism

Corresponding Author(s): Jinyu Wang,Jinli Zhang

About author:

Changjian Wang and Zhiying Yang contributed equally to this work.

Online First Date: 11 October 2022 Issue Date: 27 February 2023

Cite this article:

Xinyuan Wang,Heriberto Pfeiffer,Jiangjiang Wei, et al. Fluoride ions adsorption from water by CaCO₃ enhanced Mn–Fe mixed metal oxides[J]. Front. Chem. Sci. Eng., 2023, 17(2): 236-248.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-022-2193-8
https://academic.hep.com.cn/fcse/EN/Y2023/V17/I2/236

Fig.1 (a) XRD patterns, (b) N₂ adsorption−desorption isotherms, and (c) BJH pore-size distribution curves of the MFC and CMFC samples; (d) the pH_ZPC data of the CMFC.

Tab.1 Crystal size parameters (XRD)

Tab.2 Textural parameters of samples obtained by BET and BJH models from the N₂ adsorption–desorption technique

Fig.2 SEM images of (a) the MFC and (b) CMFC samples; (c–e) HRTEM images and (f) EDX mapping results for the CMFC sample.

Fig.3 (a) XRD pattern, (b) secondary electron images and (c) EDX mapping results for the FCMFC sample.

Tab.3 Fluoride ion adsorption capacity of various adsorbents reported in literature

Fig.4 Effects of (a) CMFC concentration, (b) the initial pH value, and (c) coexisting metal ions on fluoride ion adsorption; (d) fluoride ion adsorption performance of CMFC during five adsorption–regeneration cycles.

Fig.5 (a) Fluoride ion adsorption isotherms on CMFC samples (adsorbent dosage = 0.5 g?L^?1, T = 298 K, contact time = 24 h, pH = 7), and (b) Langmuir and (c) Freundlich isothermal modeling; (d) adsorption kinetics of CMFC samples towards fluoride ion (adsorbent dosage = 0.5 g?L^?1, initial fluoride ion concentration = 100 mg?L^?1, T = 298 K, pH = 7), and (e) pseudo-first-order and (f) pseudo-second-order fitting models.

Tab.4 Parameters of the Langmuir and Freundlich isothermal models for fluoride ion adsorption on the CMFC sample

Tab.5 Fluoride ion adsorption kinetics parameters of pseudo-first- and pseudo-second-order kinetics models

Fig.6 FTIR spectra of the initial samples (MFC and CMFC), and the sample after the fluoride ion adsorption process (FCMFC).

Fig.7 (a) XPS survey spectra of the CMFC and FCMFC samples; (b) XPS F 1s spectrum of the CMFC after fluoride ion adsorption; XPS (c) O 1s, (d) Ca 2p, (e) Mn 2p, and (f) Fe 2p spectra of the CMFC sample, before and after fluoride ion adsorption.

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