Janus multi-responsive superparamagnetic nanoparticles functionalized with two on-demand and independently cleavable ligands for Actinide separation

Kunzhou Wang; Bin Wang; Huailiang Li; Xianguo Tuo; Kun Xiong; Minhao Yan; Jérémie Courtois

doi:10.1016/j.jcis.2018.12.026

Janus multi-responsive superparamagnetic nanoparticles functionalized with two on-demand and independently cleavable ligands for Actinide separation

J Colloid Interface Sci. 2019 Mar 7:538:546-558. doi: 10.1016/j.jcis.2018.12.026. Epub 2018 Dec 7.

Authors

Kunzhou Wang¹, Bin Wang¹, Huailiang Li², Xianguo Tuo², Kun Xiong¹, Minhao Yan³, Jérémie Courtois⁴

Affiliations

¹ State Key Laboratory of Environment-friendly Energy Materials, Southwest University of Science and Technology, Mianyang 621010, China.
² Fundamental Science on Nuclear Wastes and Environmental Safety Laboratory, Southwest University of Science and Technology, Mianyang 621010, China.
³ State Key Laboratory of Environment-friendly Energy Materials, Southwest University of Science and Technology, Mianyang 621010, China. Electronic address: yanminhao@swust.edu.cn.
⁴ State Key Laboratory of Environment-friendly Energy Materials, Southwest University of Science and Technology, Mianyang 621010, China. Electronic address: jeremiecourtois@swust.edu.cn.

PMID: 30553088
DOI: 10.1016/j.jcis.2018.12.026

Abstract

Hypothesis: Nanoparticles functionalized with ligands which can on-demand and remotely be detached have recently attracted interest as stimuli-responsive materials. Research is now focused on multi-responsive systems, with applications in environmental science and biomedicine. The possibility to covalently couple two different ligands on a single nanoparticles, and to release them independently is investigated. This concept of nanoparticles functionalized with dual on-demand cleavable ligands is exploited in ground water decontamination and radionuclides separation. Efficient separation of contaminants in a single step is expected, simplifying partitioning process and decreasing generation of secondary waste by nuclear industry.

Experiments: Sub-10 nm Janus superparamagnetic nanoparticles are functionalized by click-chemistry (thiol and Diels-Alder) with two different Actinide-specific chelators. The reversible covalent bonds allow to detach chelators independently by either pH- or thermo-stimulation. The nanoparticles decorated with diethylenetriamine-pentaacetic acid (DTPA) and [(2-furan-2-yl-2-hydroxy-ethylcarbamoyl)-methoxy]-acetic acid (FHECMAA) are incubated with UO₂²⁺ and La³⁺ (as substitute for Pu³⁺) at pH = 3 and 7 before chelator-metal complexes are released. Metal contents are measured to determine separation efficiency.

Findings: Chelators can be detached from Janus nanoparticles with perfect selectivity. The nanoparticles are highly efficient for extraction of metals in acidic medium and show good ability for separation of U and La at neutral pH.

Keywords: Actinide separation; Multi-responsive; Nanoparticles; Responsivity; Reversible covalent bond; Surface functionalization; Thermo-responsive; Water treatment; pH-responsive.