Mechanistic study on boron adsorption and isotopic separation with magnetic magnetite nanoparticles
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Mechanistic study on boron adsorption and isotopic separation with magnetic magnetite nanoparticles Tao Chen1,2, Jiafei Lyu1,2, Qingfeng Wang1,2, Peng Bai1,2, Ying Wu3, and Xianghai Guo1,2,4,*
1
Department of Pharmaceutical Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China 2 Key Laboratory of Systems Bioengineering (Ministry of Education), Tianjin University, Tianjin 300072, China 3 The School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, Guangdong, China 4 School of Marine Science and Technology, Tianjin University, Tianjin 300072, China
Received: 22 June 2020
ABSTRACT
Accepted: 4 November 2020
Good boron removal and isotopic separation behavior was observed on magnetic magnetite nanoparticles (MMNs) in a previous study, but the mechanism of boron adsorption and isotopic separation remains unclear. Here, experimental studies accompanied by quantum chemistry calculations were implemented for the first time to reveal the nature of boron adsorption and isotopic separation on MMN. First, the fitted peaks of Fe2p of MMN by X-ray photoelectron spectrometry (XPS) before and after adsorption showed decrease in Fe(II)/Fe(III) ratio, which validated the formation of Fe–O–B interaction. Fe–O– B bond was also observed through fitted peaks of O1s and dihydroxy complexation where MMNs prefer to adsorb [B(OH)4]-(H3BO3) at pH \ = pHzpc (pH [ pHzpc) identified by the ratio of integrated peaks. ATR-FTIR revealed the hydroxyl moiety as the main adsorptive group. The selectivity of MMN toward [B(OH)4]- at pH \ = pHzpc and toward H3BO3 at pH [ pHzpc was figured out by calculating the ratio between the integrated areas of B–O bands at different pH values. As a result, the trend of adsorption capacity as well as the isotopic separation factor with pH was well illustrated. The concluded adsorption mechanism from the experiment was further verified with the simulated adsorption energies (DE) and isotopic separation factors (S) calculated by DFT quantum simulation.
Published online: 17 November 2020
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Springer Science+Business
Media, LLC, part of Springer Nature 2020
Handling Editor: Dale Huber Tao Chen and Jiafei Lyu have contributed equally to this work.
Address correspondence to E-mail: [email protected]
https://doi.org/10.1007/s10853-020-05546-x
4625
J Mater Sci (2021) 56:4624–4640
GRAPHICAL ABSTRACT
Introduction Boron is a naturally occurring element that can be found in various forms combined with oxygen and other elements in compounds such as boric acid, borate and borosilicate [1]. Excess uptake of boron is harmful to vegetation, as it reduces fruit yield [2] and influences the central nervous system and genital system of human beings [3]. Besides, the range of boron concentration between excess and deficiency is narrow; for example, sunflower could grow with 0.5 ppm boron, while 1 ppm is definitely toxic [4]. As for animals, chronic exposure of boron has been shown to cause cutaneous disorders and negatively affect t
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