| Autor: |
Huynh V; Department of Chemistry and Chemical Biology , McMaster University , Hamilton , Ontario L8S 4M1 , Canada., Jesmer AH; Department of Chemistry and Chemical Biology , McMaster University , Hamilton , Ontario L8S 4M1 , Canada., Shoaib MM; Department of Chemistry and Chemical Biology , McMaster University , Hamilton , Ontario L8S 4M1 , Canada., Wylie RG; Department of Chemistry and Chemical Biology , McMaster University , Hamilton , Ontario L8S 4M1 , Canada. |
| Jazyk: |
angličtina |
| Zdroj: |
Langmuir : the ACS journal of surfaces and colloids [Langmuir] 2019 Feb 05; Vol. 35 (5), pp. 1631-1641. Date of Electronic Publication: 2018 Dec 31. |
| DOI: |
10.1021/acs.langmuir.8b03908 |
| Abstrakt: |
Poly(carboxybetaine) (pCB) hydrogels do not elicit a foreign body response due to their low-fouling properties, making them ideal implantable materials for in vivo drug and cell delivery. Current reported pCB hydrogels are cross-linked using cytotoxic UV-initiated radical polymerization limiting clinical and in vivo translation. For clinical translation, we require in situ and biorthogonal cross-linking of pCB hydrogels that are both low-fouling and low-swelling to limit nonspecific interactions and minimize tissue damage, respectively. To this end, we synthesized carboxybetaine (CB) random copolymers (molecular weight (MW): ∼7-33 kDa; Đ: 1.1-1.36) containing azide (pCB-azide) or strained alkyne (Dibenzocyclooctyne (DBCO); pCB-DBCO) that rapidly cross-link upon mixing. Unlike CB homopolymers and other CB copolymers studied, high DBCO content pCB-DBCO 30 (30% DBCO mole fraction) is thermoresponsive with a upper critical solution temperature (UCST; cloud point of ∼20 °C at 50 g/L) in water due to electrostatic associations. Due to the antipolyelectrolyte effect, pCB-DBCO 30 is salt-responsive and is soluble even at low temperatures in 5 M NaCl, which prevents zwitterion electrostatic associations. pCB-azide and pCB-DBCO with 0.05 to 0.16 cross-linker mole fractions rapidly formed 10 wt % hydrogels upon mixing that were low-swelling (increase of ∼10% in wet weight) while remaining low-fouling to proteins (∼10-20 μg cm -2 ) and cells, making them suitable for in vivo applications. pCB-X 31 hydrogels composed of pCB-azide 32 and pCB-DBCO 30 formed opaque gels in water and physiological conditions that shrunk to ∼70% of their original wet weight due to pCB-DBCO 30 's greater hydrophobicity and interchain electrostatic interactions, which promotes nonspecific protein adsorption (∼35 μg cm -2 ) and cell binding. Once formed, the electrostatic interactions in pCB-X 31 hydrogels are not fully reversible with heat or salt. Although, pCB-X 31 hydrogels are transparent when initially prepared in 5 M NaCl. This is the first demonstration of a thermo- and salt-responsive CB copolymer that can tune hydrogel protein and cell fouling properties. |
| Databáze: |
MEDLINE |
| Externí odkaz: |
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