Silica-based nanoarchitecture for an optimal combination of photothermal and chemodynamic therapy functions of Cu<sub>2–<i>x</i></sub>S cores with red emitting carbon dots

doi:10.1007/s11705-023-2362-4

Front. Chem. Sci. Eng.

2023, Vol. 17

Issue (12) : 2144-2155 https://doi.org/10.1007/s11705-023-2362-4

RESEARCH ARTICLE

Silica-based nanoarchitecture for an optimal combination of photothermal and chemodynamic therapy functions of Cu_2–xS cores with red emitting carbon dots

Alexey Stepanov¹(

), Svetlana Fedorenko¹, Kirill Kholin², Irek Nizameev³, Alexey Dovzhenko⁴, Rustem Zairov^1,⁴, Tatiana Gerasimova¹, Alexandra Voloshina¹, Anna Lyubina¹, Guzel Sibgatullina⁵, Dmitry Samigullin^3,⁵, Asiya Mustafina¹

¹. Arbuzov Institute of Organic and Physical Chemistry, FRC Kazan Scientific Center of RAS, Kazan 420088, Russia
². Department of Physics, Kazan National Research Technological University, Kazan 420015, Russia
³. Department of Nanotechnology in Electronics, Kazan National Research Technical University named after A.N. Tupolev-KAI, Kazan 420111, Russia
⁴. Kazan (Volga region) Federal University, Kazan 420008, Russia
⁵. Kazan Institute of Biochemistry and Biophysics, FRC Kazan Scientific Center of RAS, Kazan 420111, Russia

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Abstract

This study introduces multifunctional silica nanoparticles that exhibit both high photothermal and chemodynamic therapeutic activities, in addition to luminescence. The activity of the silica nanoparticles is derived from their plasmonic properties, which are a result of infusing the silica nanoparticles with multiple Cu_2–xS cores. This infusion process is facilitated by a recoating of the silica nanoparticles with a cationic surfactant. The key factors that enable the internal incorporation of the Cu_2–xS cores and the external deposition of red-emitting carbon dots are identified. The Cu_2–xS cores within the silica nanoparticles exhibit both self-boosting generation of reactive oxygen species and high photothermal conversion efficacy, which are essential for photothermal and chemodynamic activities. The silica nanoparticles’ small size (no more than 70 nm) and high colloidal stability are prerequisites for their cell internalization. The internalization of the red-emitting silica nanoparticles within cells is visualized using fluorescence microscopy techniques. The chemodynamic activity of the silica nanoparticles is associated with their dark cytotoxicity, and the mechanisms of cell death are evaluated using an apoptotic assay. The photothermal activity of the silica nanoparticles is demonstrated by significant cell death under near-infrared (1064 nm) irradiation.

Keywords copper sulfide nanoparticles chemodynamic therapy photothermal therapy carbon dots silica nanoparticles

Corresponding Author(s): Alexey Stepanov

Just Accepted Date: 31 August 2023 Online First Date: 03 November 2023 Issue Date: 30 November 2023

Cite this article:

Alexey Stepanov,Svetlana Fedorenko,Kirill Kholin, et al. Silica-based nanoarchitecture for an optimal combination of photothermal and chemodynamic therapy functions of Cu_2–xS cores with red emitting carbon dots[J]. Front. Chem. Sci. Eng., 2023, 17(12): 2144-2155.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-023-2362-4
https://academic.hep.com.cn/fcse/EN/Y2023/V17/I12/2144

Fig.1 (a, b) TEM images of Cu_2–xS nanoparticles and (c) their size distribution diagram.

Fig.2 Schematic demonstration of the synthetic procedures resulting in the nanoarchitectures with interior (Cu_2–xS@SiO₂-NH₂) and exterior localization of the Cu_2–xS cores (Cu_2–_xSRu@SiO₂-NH₂).

Fig.3 (a) TEM image of Cu_2–xS@SiO₂-NH₂ NPs, (b) size distribution for Cu_2–xS@SiO₂-NH₂, (c) size distribution for Cu_2–xS cores incorporated into Cu_2–xS@SiO₂-NH₂, (d) TEM image of Cu_2–xSRu@SiO₂ NPs, (e) size distribution for Cu_2–xSRu@SiO₂-NH₂, and (f) size distribution for Cu_2–xS cores incorporated into Cu_2–xSRu@SiO₂-NH₂.

Tab.1 DLS data for Cu_2–xS@SiO₂-NH₂, Cu_2–xSRu@SiO₂-NH₂ and Cu_2–xS@SiO₂NH₂-CDs aqueous colloids^a)

Fig.4 (a) Transmittance spectra of Cu_2–xS@SiO₂-NH₂ and Cu_2–xSRu@SiO₂-NH₂ in NIR region, (b) NPs (1 g?L^–1) in D₂O, (c) FTIR spectra of CDs (black) and Cu_2–xS@SiO₂-NH₂-CDs NPs (red) in KBr pellets, and (d) excitation (black) and emission spectra (red) of Cu_2–xS@SiO₂-NH₂-CDs NPs in aqueous colloids (λ_ex = 545 nm, λ_em = 613 nm) (4 × 10^?2 g·L^–1).

Fig.5 The heating-cooling-heating curves of Cu_2–xS@SiO₂-NH₂-CDs aqueous colloids under irradiation with 1064 nm laser light (1.5 W·cm^–2) at different concentrations: (a) 0.243 g·L^–1, 1.1 mmol·L^–1 Cu; (b) 0.200 g·L^–1, 0.91 mmol·L^–1 Cu; (c) 0.12 g·L^–1, 0.54 mmol·L^–1 Cu; (d) 0.06 g·L^–1, 0.27 mmol·L^–1; (e) 0.03 g·L^–1, 0.136 mmol·L^–1 Cu (black curves refer to Cu_2–xS@SiO₂-NH₂-CDs aqueous colloids, whereas red curves refer to deionized water for comparison); (f) the elevated temperature after the irradiation for 20 min plotted vs. concentration of the aqueous Cu_2–xS@SiO₂-NH₂-CDs colloid.

Fig.6 (a) ESR spectra of DMPO-OH? and DMPO-R? adducts generated by Cu_2–xS@SiO₂NH₂CDs (1, 2) and Cu_2–xS@SiO₂-NH₂ (3) just after addition of DMPO (1, 3) and after 15 min (2), the simulated spectrum of DMPO-OH? (sim), (b) cellular uptake of Cu_2–xS@SiO₂-NH₂-CDs (designated as Nano) by M-HeLa and Chang liver cells at a concentration of 0.03 g·L^–1, * indicates p < 0.05, (c) apoptosis assay of M-HeLa incubated with Cu_2–xS@SiO₂-NH₂-CDs, (d) apoptosis assay of Chang Liver incubated with Cu_2–xS@SiO₂-NH₂-CDs, (e) apoptosis assay of M-HeLa incubated with Cu_2–xS@SiO₂-NH₂, (f) apoptosis assay of Chang Liver incubated with Cu_2–xS@SiO₂-NH₂. The scale bars illustrate the standard deviations.

Tab.2 IC₅₀-values of Cu_2–xS@SiO₂-NH₂ and Cu_2–xS@SiO₂-NH₂-CDs measured for Chang liver and M-HeLa cell lines

Fig.7 Confocal microscopy images of the M-HeLa cells incubated with Cu_2–xS@SiO₂-NH₂-CDs (designated as Nano, 0.03 g?L^–1) and DiD.

Fig.8 The cell viability of M-HeLa cells: with no NPs and irradiation (1), incubated with 0.03 g?L^–1 Cu_2–xS@SiO₂-NH₂-CDs NPs with no irradiation (2), with no NPs but after irradiation (1064 nm) for 15 (3) and 20 min (5), incubated with 0.03 g?L^–1 Cu_2–xS@SiO₂-NH₂-CDs NPs after irradiation (1064 nm) for 15 (4) and 20 min (6).

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