Differentiation of physical and chemical cross-linking in gelatin methacryloyl hydrogels

Abstract Gelatin methacryloyl (GM) hydrogels have been investigated for almost 20 years, especially for biomedical applications. Recently, strengthening effects of a sequential cross-linking procedure, whereby GM hydrogel precursor solutions are cooled before chemical cross-linking, were reported. I...

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Autores principales:	Lisa Rebers, Raffael Reichsöllner, Sophia Regett, Günter E. M. Tovar, Kirsten Borchers, Stefan Baudis, Alexander Southan
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2021
Materias:	Medicine R Science Q
Acceso en línea:	https://doaj.org/article/8bffc52ed04c4dbea87194c24b94c97c
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spelling	oai:doaj.org-article:8bffc52ed04c4dbea87194c24b94c97c2021-12-02T14:06:25ZDifferentiation of physical and chemical cross-linking in gelatin methacryloyl hydrogels10.1038/s41598-021-82393-z2045-2322https://doaj.org/article/8bffc52ed04c4dbea87194c24b94c97c2021-02-01T00:00:00Zhttps://doi.org/10.1038/s41598-021-82393-zhttps://doaj.org/toc/2045-2322Abstract Gelatin methacryloyl (GM) hydrogels have been investigated for almost 20 years, especially for biomedical applications. Recently, strengthening effects of a sequential cross-linking procedure, whereby GM hydrogel precursor solutions are cooled before chemical cross-linking, were reported. It was hypothesized that physical and enhanced chemical cross-linking of the GM hydrogels contribute to the observed strengthening effects. However, a detailed investigation is missing so far. In this contribution, we aimed to reveal the impact of physical and chemical cross-linking on strengthening of sequentially cross-linked GM and gelatin methacryloyl acetyl (GMA) hydrogels. We investigated physical and chemical cross-linking of three different GM(A) derivatives (GM10, GM2A8 and GM2), which provided systematically varied ratios of side-group modifications. GM10 contained the highest methacryloylation degree (DM), reducing its ability to cross-link physically. GM2 had the lowest DM and showed physical cross-linking. The total modification degree, determining the physical cross-linking ability, of GM2A8 was comparable to that of GM10, but the chemical cross-linking ability was comparable to GM2. At first, we measured the double bond conversion (DBC) kinetics during chemical GM(A) cross-linking quantitatively in real-time via near infrared spectroscopy-photorheology and showed that the DBC decreased due to sequential cross-linking. Furthermore, results of circular dichroism spectroscopy and differential scanning calorimetry indicated gelation and conformation changes, which increased storage moduli of all GM(A) hydrogels due to sequential cross-linking. The data suggested that the total cross-link density determines hydrogel stiffness, regardless of the physical or chemical nature of the cross-links.Lisa RebersRaffael ReichsöllnerSophia RegettGünter E. M. TovarKirsten BorchersStefan BaudisAlexander SouthanNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 11, Iss 1, Pp 1-12 (2021)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q Lisa Rebers Raffael Reichsöllner Sophia Regett Günter E. M. Tovar Kirsten Borchers Stefan Baudis Alexander Southan Differentiation of physical and chemical cross-linking in gelatin methacryloyl hydrogels
description	Abstract Gelatin methacryloyl (GM) hydrogels have been investigated for almost 20 years, especially for biomedical applications. Recently, strengthening effects of a sequential cross-linking procedure, whereby GM hydrogel precursor solutions are cooled before chemical cross-linking, were reported. It was hypothesized that physical and enhanced chemical cross-linking of the GM hydrogels contribute to the observed strengthening effects. However, a detailed investigation is missing so far. In this contribution, we aimed to reveal the impact of physical and chemical cross-linking on strengthening of sequentially cross-linked GM and gelatin methacryloyl acetyl (GMA) hydrogels. We investigated physical and chemical cross-linking of three different GM(A) derivatives (GM10, GM2A8 and GM2), which provided systematically varied ratios of side-group modifications. GM10 contained the highest methacryloylation degree (DM), reducing its ability to cross-link physically. GM2 had the lowest DM and showed physical cross-linking. The total modification degree, determining the physical cross-linking ability, of GM2A8 was comparable to that of GM10, but the chemical cross-linking ability was comparable to GM2. At first, we measured the double bond conversion (DBC) kinetics during chemical GM(A) cross-linking quantitatively in real-time via near infrared spectroscopy-photorheology and showed that the DBC decreased due to sequential cross-linking. Furthermore, results of circular dichroism spectroscopy and differential scanning calorimetry indicated gelation and conformation changes, which increased storage moduli of all GM(A) hydrogels due to sequential cross-linking. The data suggested that the total cross-link density determines hydrogel stiffness, regardless of the physical or chemical nature of the cross-links.
format	article
author	Lisa Rebers Raffael Reichsöllner Sophia Regett Günter E. M. Tovar Kirsten Borchers Stefan Baudis Alexander Southan
author_facet	Lisa Rebers Raffael Reichsöllner Sophia Regett Günter E. M. Tovar Kirsten Borchers Stefan Baudis Alexander Southan
author_sort	Lisa Rebers
title	Differentiation of physical and chemical cross-linking in gelatin methacryloyl hydrogels
title_short	Differentiation of physical and chemical cross-linking in gelatin methacryloyl hydrogels
title_full	Differentiation of physical and chemical cross-linking in gelatin methacryloyl hydrogels
title_fullStr	Differentiation of physical and chemical cross-linking in gelatin methacryloyl hydrogels
title_full_unstemmed	Differentiation of physical and chemical cross-linking in gelatin methacryloyl hydrogels
title_sort	differentiation of physical and chemical cross-linking in gelatin methacryloyl hydrogels
publisher	Nature Portfolio
publishDate	2021
url	https://doaj.org/article/8bffc52ed04c4dbea87194c24b94c97c
work_keys_str_mv	AT lisarebers differentiationofphysicalandchemicalcrosslinkingingelatinmethacryloylhydrogels AT raffaelreichsollner differentiationofphysicalandchemicalcrosslinkingingelatinmethacryloylhydrogels AT sophiaregett differentiationofphysicalandchemicalcrosslinkingingelatinmethacryloylhydrogels AT gunteremtovar differentiationofphysicalandchemicalcrosslinkingingelatinmethacryloylhydrogels AT kirstenborchers differentiationofphysicalandchemicalcrosslinkingingelatinmethacryloylhydrogels AT stefanbaudis differentiationofphysicalandchemicalcrosslinkingingelatinmethacryloylhydrogels AT alexandersouthan differentiationofphysicalandchemicalcrosslinkingingelatinmethacryloylhydrogels
_version_	1718392033198997504

Differentiation of physical and chemical cross-linking in gelatin methacryloyl hydrogels

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