A deep understanding of the self-assembly and colloidal stability of light and pH dual-responsive spiropyran random copolymer micelle-like nano-aggregates

Espinola-Portilla, Fernando; d’Orlyé, Fanny; Gutiérrez-Granados, Silvia; Ramírez-García, Gonzalo; Varenne, Anne

doi:10.1016/j.mtcomm.2022.103499

Cited by 5 publications

(9 citation statements)

References 58 publications

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“…When combining UV light and pH 6.0 stimuli, the TEM image (Figure C) clearly shows the micelle disaggregation with a polydisperse size distribution (200–400 nm). As reported before, this result confirms that the two effects, swelling and disaggregation, can be controlled by the pH change and UV irradiation.…”

Section: Resultssupporting

confidence: 91%

“…Figure 3A shows the electropherograms of Mic and DoxHCl 1 μM in 25 mM PBS (pH 7.4), identifying a single peak for each sample. The electrophoretic mobility of Mic was calculated at −11 ± 1 × 10 −5 cm 2 V −1 s −1 , which is coherent with previous reports, 29 with a negative value due to the pK a (between 6 and 7) of SPMA molecule. 40 DoxHCl electrophoretic mobility, evaluated at +8 ± 0.5 × 10 −5 cm 2 V −1 s −1 , is coherent with its first pK a at 8.2, 41 due to the amino group.…”

Section: Electrophoretic Separations Forsupporting

confidence: 91%

“…Thereby, this work aims to obtain a deep understanding of the interactions between micelle-like aggregates and the doxorubicin model-drug. For this purpose, stimuli-responsive poly[( N -isopropylacrylamide)- co -(1′-(2-methacryloxyethyl)-3′,3′-dimethyl-6-nitro-spiro(2 H -1-benzo-pyran-2,2′-indoline)] (Poly(NIPAM- co -SPMA)) copolymer nanocarriers were synthesized, and the loading and release of poorly and highly water-soluble doxorubicin forms (Dox and Dox-HCl, respectively) were evaluated upon UV light irradiation and/or pH decrease down from 7.4 to 6.0. Capillary zone electrophoresis coupled to a fluorescence detector (CE-LIF) allowed to separate and specifically characterize the micelle-like aggregates and free doxorubicin and to quantify the loading and release capacity of the nanocarrier.…”

Section: Introductionmentioning

confidence: 99%

“…The involved structures can be seen in our previous article. 29 However, until now, the drug-loading and release capacity of those nanocarriers has been evaluated through classical methodologies based on UV−vis, fluorescence spectroscopy, and HPLC. 30−38 Unfortunately, those analytical techniques did not reveal information about interactions between the model drugs and the structural components of the micelles.…”

Section: ■ Introductionmentioning

confidence: 99%

“…Furthermore, electrostatic repulsions among the hydrophobic SP-copolymer chains are induced upon a decrease in pH and with ring protonation, triggering a structural swelling and the consequent release of antineoplastic drugs. The involved structures can be seen in our previous article . However, until now, the drug-loading and release capacity of those nanocarriers has been evaluated through classical methodologies based on UV–vis, fluorescence spectroscopy, and HPLC. − Unfortunately, those analytical techniques did not reveal information about interactions between the model drugs and the structural components of the micelles.…”

Section: Introductionmentioning

confidence: 99%

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Rational Understanding of Loading and Release of Doxorubicin by UV-Light- and pH-Responsive Poly(NIPAM-co-SPMA) Micelle-like Aggregates

et al. 2022

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A deep understanding of the interactions between micelle-like aggregates and antineoplastic drugs is paramount to control their adequate delivery. Herein, Poly(NIPAM-co-SPMA) copolymer nanocarriers were synthesized according to our previous published methodology, and the loading and release of poorly and highly water-soluble doxorubicin forms (Dox and Dox-HCl, respectively) were evaluated upon UV light irradiation and pH-variation stimuli. Capillary electrophoresis (CE) coupled to a fluorescence detector (LIF) allowed us to specifically characterize these systems and deeply study the loading and release processes. For this purpose, varying concentrations of doxorubicin were tested, and the loading/release rates were indirectly quantified thanks to the "free" doxorubicin concentration in solution. This study highlighted that Dox loading (9.4 μg/mg) was more effective than Dox-HCl loading (5.5 μg/mg). In contrast, 68 and 74% of Dox-HCl were respectively released after 2 min upon pH variation (from 7.4 to 6.0) and combined UV + pH 6.0 stimuli, while only 27% of Dox was invariably released upon application of the same stimuli. These results are coherent with the characteristics of both DoxHCl and Dox: Electrostatic interactions between Dox-HCl and the micelle-membrane structure (NIPAM) seemed predominant, while hydrophobic interactions were expected between Dox and the SP moieties at the inner part of the micelle-like aggregate, leading to different behaviors in both loading and release of the two doxorubicin forms. For doxorubicin loading concentrations higher than 3 μM, the electrophoretic profiles presented an additional peak. Thanks to CE characterizations, this peak was attributed to the formation of a complex formed between the nonaggregated copolymer and the doxorubicin molecules. This report therefore undergoes deep characterization of the dynamic formation of different micelle/drug complexes involved in the global drug-delivery behavior and therefore contributes to the development of more effective stimuli-responsive nanocarriers.

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Section: Resultssupporting

confidence: 91%

Section: Electrophoretic Separations Forsupporting

confidence: 91%

Section: Introductionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%