19F NMR Relaxometry and Diffusometry for Measuring Cargo Molecule Dynamics in GelMA Hydrogels
Abstract Understanding payload diffusion is an important topic in hydrogel drug delivery. While proton nuclear magnetic resonance (NMR) spectroscopy allows for direct examination of water dynamics in hydrogels, it is challenging to study the dynamics of payloads due to spectral crowding and distorti...
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Wiley-VCH
2025-08-01
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| Series: | Macromolecular Materials and Engineering |
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| Online Access: | https://doi.org/10.1002/mame.202400348 |
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| author | Chun‐Wei Chang Bronwin L. Dargaville Konstantin I. Momot Dietmar W. Hutmacher |
| author_facet | Chun‐Wei Chang Bronwin L. Dargaville Konstantin I. Momot Dietmar W. Hutmacher |
| author_sort | Chun‐Wei Chang |
| collection | DOAJ |
| description | Abstract Understanding payload diffusion is an important topic in hydrogel drug delivery. While proton nuclear magnetic resonance (NMR) spectroscopy allows for direct examination of water dynamics in hydrogels, it is challenging to study the dynamics of payloads due to spectral crowding and distortions. Fluorine‐19, not biologically endogenous in humans and having high NMR receptivity, can be easily incorporated into molecules of interest and therefore used as an alternative probe for dynamics of payload molecules in hydrogels. In this study, the dynamics of fluorine‐containing compounds trifluoroethylamine (TFEA, a small molecule), ciprofloxacin (CF, a medium‐size molecule), and fluorinated lysozyme (FL, a ≈15 kDa protein) are measured both in solution and gelatin methacrylate (GelMA) hydrogels. For each payload molecule, the rotational correlation time and translational diffusion coefficient, as well as the effective microviscosity of the media, are measured. Spin‐spin relaxation (T2) is also used to probe chemical exchange as an indicator of payload–polymer interactions. The in situ interaction between payload and polymer network and precise characterization of payload dynamics within hydrogels show that fluorine‐19 nuclear magnetic resonance (19F NMR) relaxometry and diffusometry are important techniques in hydrogel drug delivery and, more generally, in biomaterial science, tissue engineering, and regenerative medicine. |
| format | Article |
| id | doaj-art-340d7644618a42e2bbf38cc4bfbb965b |
| institution | Kabale University |
| issn | 1438-7492 1439-2054 |
| language | English |
| publishDate | 2025-08-01 |
| publisher | Wiley-VCH |
| record_format | Article |
| series | Macromolecular Materials and Engineering |
| spelling | doaj-art-340d7644618a42e2bbf38cc4bfbb965b2025-08-20T08:39:24ZengWiley-VCHMacromolecular Materials and Engineering1438-74921439-20542025-08-013108n/an/a10.1002/mame.20240034819F NMR Relaxometry and Diffusometry for Measuring Cargo Molecule Dynamics in GelMA HydrogelsChun‐Wei Chang0Bronwin L. Dargaville1Konstantin I. Momot2Dietmar W. Hutmacher3Max Planck Queensland Centre on the Materials Science for Extracellular Matrices Queensland University of Technology (QUT) Brisbane QLD 4059 AustraliaMax Planck Queensland Centre on the Materials Science for Extracellular Matrices Queensland University of Technology (QUT) Brisbane QLD 4059 AustraliaSchool of Chemistry and Physics Queensland University of Technology (QUT) Brisbane QLD 4001 AustraliaMax Planck Queensland Centre on the Materials Science for Extracellular Matrices Queensland University of Technology (QUT) Brisbane QLD 4059 AustraliaAbstract Understanding payload diffusion is an important topic in hydrogel drug delivery. While proton nuclear magnetic resonance (NMR) spectroscopy allows for direct examination of water dynamics in hydrogels, it is challenging to study the dynamics of payloads due to spectral crowding and distortions. Fluorine‐19, not biologically endogenous in humans and having high NMR receptivity, can be easily incorporated into molecules of interest and therefore used as an alternative probe for dynamics of payload molecules in hydrogels. In this study, the dynamics of fluorine‐containing compounds trifluoroethylamine (TFEA, a small molecule), ciprofloxacin (CF, a medium‐size molecule), and fluorinated lysozyme (FL, a ≈15 kDa protein) are measured both in solution and gelatin methacrylate (GelMA) hydrogels. For each payload molecule, the rotational correlation time and translational diffusion coefficient, as well as the effective microviscosity of the media, are measured. Spin‐spin relaxation (T2) is also used to probe chemical exchange as an indicator of payload–polymer interactions. The in situ interaction between payload and polymer network and precise characterization of payload dynamics within hydrogels show that fluorine‐19 nuclear magnetic resonance (19F NMR) relaxometry and diffusometry are important techniques in hydrogel drug delivery and, more generally, in biomaterial science, tissue engineering, and regenerative medicine.https://doi.org/10.1002/mame.202400348fluorine‐19 nuclear magnetic resonance (NMR) spectroscopygelatin methacrylatehydrogel drug delivery system (DDS)relaxometry |
| spellingShingle | Chun‐Wei Chang Bronwin L. Dargaville Konstantin I. Momot Dietmar W. Hutmacher 19F NMR Relaxometry and Diffusometry for Measuring Cargo Molecule Dynamics in GelMA Hydrogels Macromolecular Materials and Engineering fluorine‐19 nuclear magnetic resonance (NMR) spectroscopy gelatin methacrylate hydrogel drug delivery system (DDS) relaxometry |
| title | 19F NMR Relaxometry and Diffusometry for Measuring Cargo Molecule Dynamics in GelMA Hydrogels |
| title_full | 19F NMR Relaxometry and Diffusometry for Measuring Cargo Molecule Dynamics in GelMA Hydrogels |
| title_fullStr | 19F NMR Relaxometry and Diffusometry for Measuring Cargo Molecule Dynamics in GelMA Hydrogels |
| title_full_unstemmed | 19F NMR Relaxometry and Diffusometry for Measuring Cargo Molecule Dynamics in GelMA Hydrogels |
| title_short | 19F NMR Relaxometry and Diffusometry for Measuring Cargo Molecule Dynamics in GelMA Hydrogels |
| title_sort | 19f nmr relaxometry and diffusometry for measuring cargo molecule dynamics in gelma hydrogels |
| topic | fluorine‐19 nuclear magnetic resonance (NMR) spectroscopy gelatin methacrylate hydrogel drug delivery system (DDS) relaxometry |
| url | https://doi.org/10.1002/mame.202400348 |
| work_keys_str_mv | AT chunweichang 19fnmrrelaxometryanddiffusometryformeasuringcargomoleculedynamicsingelmahydrogels AT bronwinldargaville 19fnmrrelaxometryanddiffusometryformeasuringcargomoleculedynamicsingelmahydrogels AT konstantinimomot 19fnmrrelaxometryanddiffusometryformeasuringcargomoleculedynamicsingelmahydrogels AT dietmarwhutmacher 19fnmrrelaxometryanddiffusometryformeasuringcargomoleculedynamicsingelmahydrogels |