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Biodegradable rare earth fluorochloride nanocrystals for phototheranostics† †Electronic supplementary information (ESI) available: Additional data for characterization of our Nd doped SrFCl and SrF2 nanoparticles, including the following: SEM image, steady-state and time-resolved luminescence spectra, integrated PL emission intensities and fitted decay time using single exponential fitting of SrFCl nanoparticles doped with varying Nd dopant concentration from 1 to 10 mol%; PL emission spectra and integrated emission intensities of SrFCl:Nd2 and SrF2:Nd2 NPs. Additional data for characterization of SrFCl:Nd2@PDA NPs, including TGA, FTIR, PA spectra and PA images. See DOI: 10.1039/d0ra00760a

ABSTRACT: The biodegradable Nd doped SrFCl nanoparticles coated with polydopamine (SrFCl:Nd@PDA NPs) have been demonstrated as a phototheranostic agent. Rare earth (RE) doped inorganic nanocrystals have been demonstrated as efficient contrast agents for deep tissue shortwave-infrared (SWIR) imaging with high sensitivities leading to potential early detection of tumors. However, a potential concern is the unknown long-term toxicity and incompatibility of inorganic nanocrystals. In this work, biodegradable rare earth nanocrystals of Nd doped SrFCl coated with polydopamine (SrFCl:Nd@PDA) were designed. Instead of traditional fluoride hosts, the chlorinated SrF2 (i.e. SrFCl) with low phonon energy which significantly improved the brightness of SrFCl:Nd in the SWIR region was used as the host. After coating with a NIR-absorptive PDA layer, the SrFCl:Nd nanoparticles serve as not only a contrast agent for photoacoustic imaging, but also a potential photothermal agent for cancer therapy. Moreover, these SrFCl:Nd@PDA nanoparticles can be rapidly and completely degraded in phosphate buffer solution within 1 h, which effectively addresses the concerns of the deleterious effects arising from potential long term accumulation. The increased accumulation and retention at tumor sites, and complete in vivo clearance ?6 h after injection make these SrFCl:Nd@PDA nanoparticles a promising degradable phototheranostic agent.

SUBMITTER: Zhao X

PROVIDER: S-EPMC7497408 | biostudies-literature | 2020 Apr

REPOSITORIES: biostudies-literature

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Project description:Rare-earth labeling in biological apatite could provide critical information for the pathologic transition (osteoclastic) and physiologic regeneration (osteogenesis) of bone and teeth because of their characteristic site-sensitive fluorescence in different coordinative conditions of various tissues in many biological processes. However, the rare-earth labeling method for biological apatites, i.e., carbonated-hydroxyapatite, has been rarely found in the literature. In this paper, we report a Pourbaix-diagram guided mineralizing strategy to controllable carbonation and doping of rare-earth ions in the hydroxyapatite (HA) lattice. The carbonation process of hydroxyapatite was achieved by controllable mineralization in hydrothermal condition with K2CO3 as the carbonate source, which results into the pure B-type carbonated hydroxyapatite (CHA) with tunable carbonate substitution degree. All of the as-synthesized materials crystalized into P63/m (No. 176) space group with the lattice parameter of a decreases and c increases with the increasing of carbonate content in the reactants. Structural refinement results revealed that the substitution of planar CO32- is superimposed on one of the faces of PO43- tetrahedral sub-units with a rotation angle of 30° in reference to c-axis. All of the hydrothermally synthesized CHA nanocrystals show hexagonal rod-like morphology with the length of 70-110 nm and diameter of 21-35 nm, and the decreasing length/diameter ratio from 3.61 to 2.96 from low to high carbonated level of the samples. Five rare-earth cations, of Pr3+, Sm3+, Eu3+, Tb3+, and Ho3+, were used as possible probe ions that can be doped into either HA or CHA lattice. The site-preference of Tb3+ doping is the same in the crystallographic site of HA and CHA according to characteristic emission peaks of 5D4-7Fj (j = 3-6) transitions in their photoluminescent spectroscopy. Our work provides a controllable carbonation method for rare-earth labeling hydroxyapatite nanomaterials with potential biologically active implant powders for bone repair and tissue regeneration.

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