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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MDPI AG
2024-03-01
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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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