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An entropy–elastic gelatin-based hydrogel system
Gelatin is a non-immunogenic and degradable biopolymer, which is widely applied in the biomedical field e.g. for drug capsules or as absorbable hemostats. However, gelatin materials present limited and hardly reproducible mechanical properties especially in aqueous systems, particularly caused by th...
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Published in: | Journal of materials chemistry 2010-10, Vol.20 (40), p.8875-8884 |
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creator | Tronci, Giuseppe Neffe, Axel Thomas Pierce, Benjamin Franklin Lendlein, Andreas |
description | Gelatin is a non-immunogenic and degradable biopolymer, which is widely applied in the biomedical field e.g. for drug capsules or as absorbable hemostats. However, gelatin materials present limited and hardly reproducible mechanical properties especially in aqueous systems, particularly caused by the uncontrollable partial renaturation of collagen-like triple helices. Therefore, mechanically demanding applications for gelatin-based materials, such as vascular patches, i.e. hydrogel films that seal large incisions in vessel walls, and for induced autoregeneration, are basically excluded if this challenge is not addressed. Through the synthesis of a defined chemical network of gelatin with hexamethylene diisocyanate (HDI) in DMSO, the self-organization of gelatin chains could be hindered and amorphous gelatin films were successfully prepared having Young's moduli of 60-530 kPa. Transferring the crosslinking reaction with HDI and, alternatively, ethyl lysine diisocyanate (LDI), to water as reaction medium allowed the tailoring of swelling behaviour and mechanical properties by variation of crosslinker content while suppressing the formation of helices. The hydrogels had Young's moduli of 70-740 kPa, compressive moduli of 16-48 kPa, and degrees of swelling of 300-800 vol%. Test reactions investigated by ESI mass spectrometry allowed the identification and quantification of reaction products of the crosslinking reaction. The HDI crosslinked networks were stabilized by direct covalent crosslinks (ca. 10 mol%), supported by grafting (50 mol%) and blending of hydrophobic oligomeric chains. For the LDI-based networks, less crosslinked (3 mol%) and grafted species (5 mol%) and much higher amounts of oligomers were observed. The adjustable hydrogel system enables the application of gelatin-based materials in physiological environments. |
doi_str_mv | 10.1039/c0jm00883d |
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However, gelatin materials present limited and hardly reproducible mechanical properties especially in aqueous systems, particularly caused by the uncontrollable partial renaturation of collagen-like triple helices. Therefore, mechanically demanding applications for gelatin-based materials, such as vascular patches, i.e. hydrogel films that seal large incisions in vessel walls, and for induced autoregeneration, are basically excluded if this challenge is not addressed. Through the synthesis of a defined chemical network of gelatin with hexamethylene diisocyanate (HDI) in DMSO, the self-organization of gelatin chains could be hindered and amorphous gelatin films were successfully prepared having Young's moduli of 60-530 kPa. Transferring the crosslinking reaction with HDI and, alternatively, ethyl lysine diisocyanate (LDI), to water as reaction medium allowed the tailoring of swelling behaviour and mechanical properties by variation of crosslinker content while suppressing the formation of helices. The hydrogels had Young's moduli of 70-740 kPa, compressive moduli of 16-48 kPa, and degrees of swelling of 300-800 vol%. Test reactions investigated by ESI mass spectrometry allowed the identification and quantification of reaction products of the crosslinking reaction. The HDI crosslinked networks were stabilized by direct covalent crosslinks (ca. 10 mol%), supported by grafting (50 mol%) and blending of hydrophobic oligomeric chains. For the LDI-based networks, less crosslinked (3 mol%) and grafted species (5 mol%) and much higher amounts of oligomers were observed. 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However, gelatin materials present limited and hardly reproducible mechanical properties especially in aqueous systems, particularly caused by the uncontrollable partial renaturation of collagen-like triple helices. Therefore, mechanically demanding applications for gelatin-based materials, such as vascular patches, i.e. hydrogel films that seal large incisions in vessel walls, and for induced autoregeneration, are basically excluded if this challenge is not addressed. Through the synthesis of a defined chemical network of gelatin with hexamethylene diisocyanate (HDI) in DMSO, the self-organization of gelatin chains could be hindered and amorphous gelatin films were successfully prepared having Young's moduli of 60-530 kPa. Transferring the crosslinking reaction with HDI and, alternatively, ethyl lysine diisocyanate (LDI), to water as reaction medium allowed the tailoring of swelling behaviour and mechanical properties by variation of crosslinker content while suppressing the formation of helices. The hydrogels had Young's moduli of 70-740 kPa, compressive moduli of 16-48 kPa, and degrees of swelling of 300-800 vol%. Test reactions investigated by ESI mass spectrometry allowed the identification and quantification of reaction products of the crosslinking reaction. The HDI crosslinked networks were stabilized by direct covalent crosslinks (ca. 10 mol%), supported by grafting (50 mol%) and blending of hydrophobic oligomeric chains. For the LDI-based networks, less crosslinked (3 mol%) and grafted species (5 mol%) and much higher amounts of oligomers were observed. The adjustable hydrogel system enables the application of gelatin-based materials in physiological environments.</description><subject>Crosslinking</subject><subject>Gelatins</subject><subject>Grafting</subject><subject>Helices</subject><subject>Hydrogels</subject><subject>Mechanical properties</subject><subject>Modulus of elasticity</subject><subject>Networks</subject><subject>Swelling</subject><issn>0959-9428</issn><issn>1364-5501</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2010</creationdate><recordtype>article</recordtype><recordid>eNpFkMtKxDAYhYMoWEc3PkF3ghD901z-ZjkM3mDAja5DmqbaoTeTzKI738E39EmsjODqHA4f58Ah5JLBDQOubx3seoCy5PURyRhXgkoJ7JhkoKWmWhTlKTmLcQfAGCqZkWI95H5IYZzm788v39mYWpe_LSa1A61s9HX-PtdhXKI8zjH5_pycNLaL_uJPV-T1_u5l80i3zw9Pm_WWukLxRGvLLTDplES27KKToJRQVqFmGrXCAlB4LYQtGq5lBcjQIUoBUlWN13xFrg69Uxg_9j4m07fR-a6zgx_30ZRSIgBytZDXB9KFMcbgGzOFtrdhNgzM7y_m_xf-A9v4VK4</recordid><startdate>20101028</startdate><enddate>20101028</enddate><creator>Tronci, Giuseppe</creator><creator>Neffe, Axel Thomas</creator><creator>Pierce, Benjamin Franklin</creator><creator>Lendlein, Andreas</creator><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope></search><sort><creationdate>20101028</creationdate><title>An entropy–elastic gelatin-based hydrogel system</title><author>Tronci, Giuseppe ; Neffe, Axel Thomas ; Pierce, Benjamin Franklin ; Lendlein, Andreas</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c263t-da3a015c65714287c506646a6791979672074e944a2f395b0717c7754056bfe93</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2010</creationdate><topic>Crosslinking</topic><topic>Gelatins</topic><topic>Grafting</topic><topic>Helices</topic><topic>Hydrogels</topic><topic>Mechanical properties</topic><topic>Modulus of elasticity</topic><topic>Networks</topic><topic>Swelling</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Tronci, Giuseppe</creatorcontrib><creatorcontrib>Neffe, Axel Thomas</creatorcontrib><creatorcontrib>Pierce, Benjamin Franklin</creatorcontrib><creatorcontrib>Lendlein, Andreas</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><jtitle>Journal of materials chemistry</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Tronci, Giuseppe</au><au>Neffe, Axel Thomas</au><au>Pierce, Benjamin Franklin</au><au>Lendlein, Andreas</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>An entropy–elastic gelatin-based hydrogel system</atitle><jtitle>Journal of materials chemistry</jtitle><date>2010-10-28</date><risdate>2010</risdate><volume>20</volume><issue>40</issue><spage>8875</spage><epage>8884</epage><pages>8875-8884</pages><issn>0959-9428</issn><eissn>1364-5501</eissn><notes>ObjectType-Article-2</notes><notes>SourceType-Scholarly Journals-1</notes><notes>ObjectType-Feature-1</notes><notes>content type line 23</notes><abstract>Gelatin is a non-immunogenic and degradable biopolymer, which is widely applied in the biomedical field e.g. for drug capsules or as absorbable hemostats. However, gelatin materials present limited and hardly reproducible mechanical properties especially in aqueous systems, particularly caused by the uncontrollable partial renaturation of collagen-like triple helices. Therefore, mechanically demanding applications for gelatin-based materials, such as vascular patches, i.e. hydrogel films that seal large incisions in vessel walls, and for induced autoregeneration, are basically excluded if this challenge is not addressed. Through the synthesis of a defined chemical network of gelatin with hexamethylene diisocyanate (HDI) in DMSO, the self-organization of gelatin chains could be hindered and amorphous gelatin films were successfully prepared having Young's moduli of 60-530 kPa. Transferring the crosslinking reaction with HDI and, alternatively, ethyl lysine diisocyanate (LDI), to water as reaction medium allowed the tailoring of swelling behaviour and mechanical properties by variation of crosslinker content while suppressing the formation of helices. The hydrogels had Young's moduli of 70-740 kPa, compressive moduli of 16-48 kPa, and degrees of swelling of 300-800 vol%. Test reactions investigated by ESI mass spectrometry allowed the identification and quantification of reaction products of the crosslinking reaction. The HDI crosslinked networks were stabilized by direct covalent crosslinks (ca. 10 mol%), supported by grafting (50 mol%) and blending of hydrophobic oligomeric chains. For the LDI-based networks, less crosslinked (3 mol%) and grafted species (5 mol%) and much higher amounts of oligomers were observed. The adjustable hydrogel system enables the application of gelatin-based materials in physiological environments.</abstract><doi>10.1039/c0jm00883d</doi><tpages>10</tpages></addata></record> |
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source | Royal Society of Chemistry |
subjects | Crosslinking Gelatins Grafting Helices Hydrogels Mechanical properties Modulus of elasticity Networks Swelling |
title | An entropy–elastic gelatin-based hydrogel system |
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