Kinetically stable metal ligand charge transfer complexes as crosslinks in nanogels/hydrogels: Physical properties and cytotoxicity

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Abstract

A terpyridine end-functionalized 8-arm poly(ethylene glycol) was prepared using the reaction of a 4'-aminopentanoxy substituted terpyridine with a p-nitrophenyl chloroformate activated PEG-(OH)8. Supramolecular complexation of the polymer terpyridine moieties by Fe2+ ions was investigated using NMR, UV-Vis and dynamic light scattering experiments. At low concentrations addition of Fe2+ ions to an aqueous solution of the polymer conjugate afforded nanogels with a single size distribution around 250nm. At concentrations above 3wt%, and at a 1:2 metal to ligand molar ratio, hydrogels were formed with increasing mechanical properties at increasing polymer concentrations. Using bovine chondrocytes, the biocompatibility and potential cytotoxicity of the polymer conjugate, nanogels and hydrogels were studied. The polymer conjugate with free ligands was toxic to the cells likely due to depletion of essential metal ions. When the terpyridine groups were complexed with Fe2+ ions, both nanogel suspensions and hydrogels showed no cytotoxicity in direct contact with chondrocytes. Indirect contact of gels with chondrocytes using transwells revealed the absence of toxic components by leaching. A Live-Dead assay on chondrocytes encapsulated in the hydrogels indicated that the hydrogels are cytocompatible, revealing the potential use of these materials for biomedical and pharmaceutical applications.
Original languageEnglish
Pages (from-to)136-144
JournalActa biomaterialia
Volume15
DOIs
Publication statusPublished - 17 Aug 2015

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Hydrogels
Cytotoxicity
Charge transfer
Chondrocytes
Polymers
Physical properties
Metals
Ligands
Ions
Poisons
Polyethylene glycols
Ethylene Glycol
Dynamic light scattering
Complexation
Biocompatibility
Drug products
Leaching
Metal ions
Assays
Suspensions

Keywords

  • IR-97123
  • METIS-311632

Cite this

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title = "Kinetically stable metal ligand charge transfer complexes as crosslinks in nanogels/hydrogels: Physical properties and cytotoxicity",
abstract = "A terpyridine end-functionalized 8-arm poly(ethylene glycol) was prepared using the reaction of a 4'-aminopentanoxy substituted terpyridine with a p-nitrophenyl chloroformate activated PEG-(OH)8. Supramolecular complexation of the polymer terpyridine moieties by Fe2+ ions was investigated using NMR, UV-Vis and dynamic light scattering experiments. At low concentrations addition of Fe2+ ions to an aqueous solution of the polymer conjugate afforded nanogels with a single size distribution around 250nm. At concentrations above 3wt{\%}, and at a 1:2 metal to ligand molar ratio, hydrogels were formed with increasing mechanical properties at increasing polymer concentrations. Using bovine chondrocytes, the biocompatibility and potential cytotoxicity of the polymer conjugate, nanogels and hydrogels were studied. The polymer conjugate with free ligands was toxic to the cells likely due to depletion of essential metal ions. When the terpyridine groups were complexed with Fe2+ ions, both nanogel suspensions and hydrogels showed no cytotoxicity in direct contact with chondrocytes. Indirect contact of gels with chondrocytes using transwells revealed the absence of toxic components by leaching. A Live-Dead assay on chondrocytes encapsulated in the hydrogels indicated that the hydrogels are cytocompatible, revealing the potential use of these materials for biomedical and pharmaceutical applications.",
keywords = "IR-97123, METIS-311632",
author = "Rong Wang and Both, {Sanne Karijn} and M. Geven and L. Calucci and C. Forte and Dijkstra, {Pieter J.} and Karperien, {Hermanus Bernardus Johannes}",
year = "2015",
month = "8",
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doi = "10.1016/j.actbio.2015.08.019",
language = "English",
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journal = "Acta biomaterialia",
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publisher = "Elsevier",

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TY - JOUR

T1 - Kinetically stable metal ligand charge transfer complexes as crosslinks in nanogels/hydrogels: Physical properties and cytotoxicity

AU - Wang, Rong

AU - Both, Sanne Karijn

AU - Geven, M.

AU - Calucci, L.

AU - Forte, C.

AU - Dijkstra, Pieter J.

AU - Karperien, Hermanus Bernardus Johannes

PY - 2015/8/17

Y1 - 2015/8/17

N2 - A terpyridine end-functionalized 8-arm poly(ethylene glycol) was prepared using the reaction of a 4'-aminopentanoxy substituted terpyridine with a p-nitrophenyl chloroformate activated PEG-(OH)8. Supramolecular complexation of the polymer terpyridine moieties by Fe2+ ions was investigated using NMR, UV-Vis and dynamic light scattering experiments. At low concentrations addition of Fe2+ ions to an aqueous solution of the polymer conjugate afforded nanogels with a single size distribution around 250nm. At concentrations above 3wt%, and at a 1:2 metal to ligand molar ratio, hydrogels were formed with increasing mechanical properties at increasing polymer concentrations. Using bovine chondrocytes, the biocompatibility and potential cytotoxicity of the polymer conjugate, nanogels and hydrogels were studied. The polymer conjugate with free ligands was toxic to the cells likely due to depletion of essential metal ions. When the terpyridine groups were complexed with Fe2+ ions, both nanogel suspensions and hydrogels showed no cytotoxicity in direct contact with chondrocytes. Indirect contact of gels with chondrocytes using transwells revealed the absence of toxic components by leaching. A Live-Dead assay on chondrocytes encapsulated in the hydrogels indicated that the hydrogels are cytocompatible, revealing the potential use of these materials for biomedical and pharmaceutical applications.

AB - A terpyridine end-functionalized 8-arm poly(ethylene glycol) was prepared using the reaction of a 4'-aminopentanoxy substituted terpyridine with a p-nitrophenyl chloroformate activated PEG-(OH)8. Supramolecular complexation of the polymer terpyridine moieties by Fe2+ ions was investigated using NMR, UV-Vis and dynamic light scattering experiments. At low concentrations addition of Fe2+ ions to an aqueous solution of the polymer conjugate afforded nanogels with a single size distribution around 250nm. At concentrations above 3wt%, and at a 1:2 metal to ligand molar ratio, hydrogels were formed with increasing mechanical properties at increasing polymer concentrations. Using bovine chondrocytes, the biocompatibility and potential cytotoxicity of the polymer conjugate, nanogels and hydrogels were studied. The polymer conjugate with free ligands was toxic to the cells likely due to depletion of essential metal ions. When the terpyridine groups were complexed with Fe2+ ions, both nanogel suspensions and hydrogels showed no cytotoxicity in direct contact with chondrocytes. Indirect contact of gels with chondrocytes using transwells revealed the absence of toxic components by leaching. A Live-Dead assay on chondrocytes encapsulated in the hydrogels indicated that the hydrogels are cytocompatible, revealing the potential use of these materials for biomedical and pharmaceutical applications.

KW - IR-97123

KW - METIS-311632

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DO - 10.1016/j.actbio.2015.08.019

M3 - Article

VL - 15

SP - 136

EP - 144

JO - Acta biomaterialia

JF - Acta biomaterialia

SN - 1742-7061

ER -