pH-Responsive Cellulose/Silk/Fe<sub>3</sub>O<sub>4</sub> Hydrogel Microbeads Designed for Biomedical Applications

In this study, cellulose/Fe<sub>3</sub>O<sub>4</sub> hydrogel microbeads were prepared through the sol–gel transition of a solvent-in-oil emulsion using various cellulose-dissolving solvents and soybean oil without surfactants. Particularly, 40% tetrabutylammonium hydroxide (...

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Main Authors: Seung Hyeon Weon, Yuhyeon Na, Jiwoo Han, Jeong Woo Lee, Hyung Joo Kim, Saerom Park, Sang Hyun Lee
Format: Article
Language:English
Published: MDPI AG 2024-03-01
Series:Gels
Subjects:
Online Access:https://www.mdpi.com/2310-2861/10/3/200
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author Seung Hyeon Weon
Yuhyeon Na
Jiwoo Han
Jeong Woo Lee
Hyung Joo Kim
Saerom Park
Sang Hyun Lee
author_facet Seung Hyeon Weon
Yuhyeon Na
Jiwoo Han
Jeong Woo Lee
Hyung Joo Kim
Saerom Park
Sang Hyun Lee
author_sort Seung Hyeon Weon
collection DOAJ
description In this study, cellulose/Fe<sub>3</sub>O<sub>4</sub> hydrogel microbeads were prepared through the sol–gel transition of a solvent-in-oil emulsion using various cellulose-dissolving solvents and soybean oil without surfactants. Particularly, 40% tetrabutylammonium hydroxide (TBAH) and 40% tetrabutylphosphonium hydroxide (TBPH) dissolved cellulose at room temperature and effectively dispersed Fe<sub>3</sub>O<sub>4</sub>, forming cellulose/Fe<sub>3</sub>O<sub>4</sub> microbeads with an average diameter of ~15 µm. Additionally, these solvents co-dissolved cellulose and silk, allowing for the manufacture of cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> hydrogel microbeads with altered surface characteristics. Owing to the negatively charged surface characteristics, the adsorption capacity of the cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads for the cationic dye crystal violet was >10 times higher than that of the cellulose/Fe<sub>3</sub>O<sub>4</sub> microbeads. When prepared with TBAH, the initial adsorption rate of bovine serum albumin (BSA) on the cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads was 18.1 times higher than that on the cellulose/Fe<sub>3</sub>O<sub>4</sub> microbeads. When preparing TBPH, the equilibrium adsorption capacity of the cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads for BSA (1.6 g/g) was 8.5 times higher than that of the cellulose/Fe<sub>3</sub>O<sub>4</sub> microbeads. The pH-dependent BSA release from the cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads prepared with TBPH revealed 6.1-fold slower initial desorption rates and 5.2-fold lower desorption amounts at pH 2.2 than those at pH 7.4. Cytotoxicity tests on the cellulose and cellulose/silk composites regenerated with TBAH and TBPH yielded nontoxic results. Therefore, cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads are considered suitable pH-responsive supports for orally administered protein pharmaceuticals.
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spelling doaj.art-29498170f6f5462fbfdd35bea2d7ae242024-03-27T13:42:42ZengMDPI AGGels2310-28612024-03-0110320010.3390/gels10030200pH-Responsive Cellulose/Silk/Fe<sub>3</sub>O<sub>4</sub> Hydrogel Microbeads Designed for Biomedical ApplicationsSeung Hyeon Weon0Yuhyeon Na1Jiwoo Han2Jeong Woo Lee3Hyung Joo Kim4Saerom Park5Sang Hyun Lee6Department of Biological Engineering, Konkuk University, Seoul 05029, Republic of KoreaDepartment of Biological Engineering, Konkuk University, Seoul 05029, Republic of KoreaDepartment of Biological Engineering, Konkuk University, Seoul 05029, Republic of KoreaDepartment of Biological Engineering, Konkuk University, Seoul 05029, Republic of KoreaDepartment of Biological Engineering, Konkuk University, Seoul 05029, Republic of KoreaDepartment of Biological Engineering, Konkuk University, Seoul 05029, Republic of KoreaDepartment of Biological Engineering, Konkuk University, Seoul 05029, Republic of KoreaIn this study, cellulose/Fe<sub>3</sub>O<sub>4</sub> hydrogel microbeads were prepared through the sol–gel transition of a solvent-in-oil emulsion using various cellulose-dissolving solvents and soybean oil without surfactants. Particularly, 40% tetrabutylammonium hydroxide (TBAH) and 40% tetrabutylphosphonium hydroxide (TBPH) dissolved cellulose at room temperature and effectively dispersed Fe<sub>3</sub>O<sub>4</sub>, forming cellulose/Fe<sub>3</sub>O<sub>4</sub> microbeads with an average diameter of ~15 µm. Additionally, these solvents co-dissolved cellulose and silk, allowing for the manufacture of cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> hydrogel microbeads with altered surface characteristics. Owing to the negatively charged surface characteristics, the adsorption capacity of the cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads for the cationic dye crystal violet was >10 times higher than that of the cellulose/Fe<sub>3</sub>O<sub>4</sub> microbeads. When prepared with TBAH, the initial adsorption rate of bovine serum albumin (BSA) on the cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads was 18.1 times higher than that on the cellulose/Fe<sub>3</sub>O<sub>4</sub> microbeads. When preparing TBPH, the equilibrium adsorption capacity of the cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads for BSA (1.6 g/g) was 8.5 times higher than that of the cellulose/Fe<sub>3</sub>O<sub>4</sub> microbeads. The pH-dependent BSA release from the cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads prepared with TBPH revealed 6.1-fold slower initial desorption rates and 5.2-fold lower desorption amounts at pH 2.2 than those at pH 7.4. Cytotoxicity tests on the cellulose and cellulose/silk composites regenerated with TBAH and TBPH yielded nontoxic results. Therefore, cellulose/silk/Fe<sub>3</sub>O<sub>4</sub> microbeads are considered suitable pH-responsive supports for orally administered protein pharmaceuticals.https://www.mdpi.com/2310-2861/10/3/200cellulosesilkmicrobeadpH responsiveprotein support
spellingShingle Seung Hyeon Weon
Yuhyeon Na
Jiwoo Han
Jeong Woo Lee
Hyung Joo Kim
Saerom Park
Sang Hyun Lee
pH-Responsive Cellulose/Silk/Fe<sub>3</sub>O<sub>4</sub> Hydrogel Microbeads Designed for Biomedical Applications
Gels
cellulose
silk
microbead
pH responsive
protein support
title pH-Responsive Cellulose/Silk/Fe<sub>3</sub>O<sub>4</sub> Hydrogel Microbeads Designed for Biomedical Applications
title_full pH-Responsive Cellulose/Silk/Fe<sub>3</sub>O<sub>4</sub> Hydrogel Microbeads Designed for Biomedical Applications
title_fullStr pH-Responsive Cellulose/Silk/Fe<sub>3</sub>O<sub>4</sub> Hydrogel Microbeads Designed for Biomedical Applications
title_full_unstemmed pH-Responsive Cellulose/Silk/Fe<sub>3</sub>O<sub>4</sub> Hydrogel Microbeads Designed for Biomedical Applications
title_short pH-Responsive Cellulose/Silk/Fe<sub>3</sub>O<sub>4</sub> Hydrogel Microbeads Designed for Biomedical Applications
title_sort ph responsive cellulose silk fe sub 3 sub o sub 4 sub hydrogel microbeads designed for biomedical applications
topic cellulose
silk
microbead
pH responsive
protein support
url https://www.mdpi.com/2310-2861/10/3/200
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