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. 2022 Jan 20:633:127849.
doi: 10.1016/j.colsurfa.2021.127849. Epub 2021 Nov 3.

Effect of hydroxychloroquine sulfate on the gelation behavior, water mobility and structure of gelatin

Hailin Wang  1 , Wei Lu  2 , Lijing Ke  1 , Yi Wang  2 , Jianwu Zhou  1 , Pingfan Rao  1
Affiliations

Effect of hydroxychloroquine sulfate on the gelation behavior, water mobility and structure of gelatin

Hailin Wang et al. Colloids Surf A Physicochem Eng Asp. .

Abstract

Hydroxychloroquine sulfate (HCQ) is a well-established antimalarial drug that has received considerable attention during the COVID-19 associated pneumonia epidemic. Gelatin is a multifunctional biomacromolecule with pharmaceutical applications and can be used to deliver HCQ. The effect of HCQ on the gelation behaviors, water mobility, and structure of gelatin was investigated to understand the interaction between the drug and its delivery carrier. The gel strength, hardness, gelling (Tg) and melting (Tm) temperatures, gelation rate (kgel), and water mobility of gelatin decreased with increasing amounts of HCQ. The addition of HCQ led to hydrogen bonding that interfered with triple helix formation in gelatin. Fourier transform infrared spectroscopy (FTIR) and X-ray diffractometer (XRD) analysis further confirmed that the interaction between HCQ and gelatin is primarily through hydrogen bonding. Atomic force microscopy (AFM) revealed that higher content of HCQ resulted in more and larger aggregates in gelatin. These results provide not only an important understanding of gelatin for drug delivery design but also a basis for the studying interactions between a drug and its delivery carrier.

Keywords: Gelatin; Gelation behavior; Hydroxychloroquine sulfate (HCQ); Interaction; Structure.

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Conflict of interest statement

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Figures

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Graphical abstract
Fig. 1
Fig. 1
Gel strength (A), hardness (B), cohesiveness (C), gumminess (D), springiness (E) and chewiness (F) of gelatin (6.67%, w/v) with different contents (0%, 1%, 3%, 5%, 7%, and 9%, w/v) of HCQ.
Fig. 2
Fig. 2
Storage modulus (Gˊ) of gelatin with different contents of HCQ upon cooling from 40 ℃ to 5 ℃ (A) and upon heating from 5 ℃ to 40 ℃ (B). Control: 6.67% gelatin (w/v); 1% HCQ, 3% HCQ, 5% HCQ, 7% HCQ, 9% HCQ (w/v): 6.67% gelatin prepared by the different contents of HCQ solutions.
Fig. 3
Fig. 3
Evolution of storage (Gˊ) and loss (G˝) modulus during cooling and gelling of gelatin with different contents of HCQ. Control: 6.67% gelatin (w/v); 1% HCQ, 3% HCQ, 5% HCQ, 7% HCQ, 9% HCQ (w/v): 6.67% gelatin prepared by the different contents of HCQ solutions.
Fig. 4
Fig. 4
FTIR spectra of gelatin with different contents of HCQ. (a), 6.67% gelatin (w/v); (b), HCQ; (c-g), 6.67% gelatin prepared by the content of 1%, 3%, 5%, 7%, 9% HCQ (w/v) solution, respectively.
Fig. 5
Fig. 5
The relaxation time curves of gelatin with different contents of HCQ. (A), Immobile water; (B), free water. Control: 6.67% gelatin (w/v); 1% HCQ, 3% HCQ, 5% HCQ, 7% HCQ, 9% HCQ (w/v): 6.67% gelatin prepared by the different contents of HCQ solutions.
Fig. 6
Fig. 6
XRD pattern of gelatin with different contents of HCQ (A) and HCQ (B). (a), 6.67% gelatin (w/v); (b), HCQ; (c-g), 6.67% gelatin prepared by the content of 1%, 3%, 5%, 7%, and 9% HCQ (w/v) solutions, respectively.
Fig. 7
Fig. 7
Nanostructure of gelatin solution at 0.0667% (w/v). A, B, C, D, E, F: gelatin contained various HCQ content (0%, 0.01%, 0.03%, 0.05%, 0.07%, and 0.09%), respectively.
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