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Layered rare-earth hydroxides as multi-modal medical imaging probes: particle size optimisation and compositional exploration

Strimaite, Margarita; Wells, Connor J.R.; Prior, Timothy J.; Stuckey, Daniel J.; Wells, Jack A.; Davies, Gemma Louise; Williams, Gareth R.

Authors

Margarita Strimaite

Connor J.R. Wells

Profile image of Tim Prior

Dr Tim Prior T.Prior@hull.ac.uk
Senior Lecturer in Inorganic Chemistry

Daniel J. Stuckey

Jack A. Wells

Gemma Louise Davies

Gareth R. Williams



Abstract

Recently, layered rare-earth hydroxides (LRHs) have received growing attention in the field of theranostics. We have previously reported the hydrothermal synthesis of layered terbium hydroxide (LTbH), which exhibited high biocompatibility, reversible uptake of a range of model drugs, and release-sensitive phosphorescence. Despite these favourable properties, LTbH particles produced by the reported method suffered from poor size-uniformity (670 ± 564 nm), and are thus not suitable for therapeutic applications. To ameliorate this issue, we first derive an optimised hydrothermal synthesis method to generate LTbH particles with a high degree of homogeneity and reproducibility, within a size range appropriate for in vivo applications (152 ± 59 nm, n = 6). Subsequently, we apply this optimised method to synthesise a selected range of LRH materials (R = Pr, Nd, Gd, Dy, Er, Yb), four of which produced particles with an average size under 200 nm (Pr, Nd, Gd, and Dy) without the need for further optimisation. Finally, we incorporate Gd and Tb into LRHs in varying molar ratios (1 : 3, 1 : 1, and 3 : 1) and assess the combined magnetic relaxivity and phosphorescence properties of the resultant LRH materials. The lead formulation, LGd1.41Tb0.59H, was demonstrated to significantly shorten the T2 relaxation time of water (r2 = 52.06 mM−1 s−1), in addition to exhibiting a strong phosphorescence signal (over twice that of the other LRH formulations, including previously reported LTbH), therefore holding great promise as a potential multi-modal medical imaging probe.

Citation

Strimaite, M., Wells, C. J., Prior, T. J., Stuckey, D. J., Wells, J. A., Davies, G. L., & Williams, G. R. (2024). Layered rare-earth hydroxides as multi-modal medical imaging probes: particle size optimisation and compositional exploration. Dalton Transactions : an international journal of inorganic chemistry, 53(19), 8429-8442. https://doi.org/10.1039/d4dt00371c

Journal Article Type Article
Acceptance Date Apr 19, 2024
Online Publication Date Apr 19, 2024
Publication Date May 21, 2024
Deposit Date Apr 30, 2024
Publicly Available Date May 1, 2024
Journal Dalton Transactions
Print ISSN 1477-9226
Electronic ISSN 1477-9234
Publisher Royal Society of Chemistry
Peer Reviewed Peer Reviewed
Volume 53
Issue 19
Pages 8429-8442
DOI https://doi.org/10.1039/d4dt00371c
Public URL https://hull-repository.worktribe.com/output/4652661

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