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Controlled degradation of low-fouling poly(oligo(ethylene glycol)methyl ether methacrylate) hydrogels
Authors:Muhammad M Shoaib  Vincent Huynh  Yousuf Shad  Rashik Ahmed  Alexander H Jesmer  Giuseppe Melacini  Ryan G Wylie
Institution:Department of Chemistry and Chemical Biology, McMaster University, Hamilton Ontario L8S 4M1 Canada.; Department of Biochemistry and Biomedical Sciences, McMaster University, Hamilton Ontario L8S 4M1 Canada ; School of Biomedical Engineering, McMaster University, Hamilton Ontario L8S 4M1 Canada
Abstract:Degradable low-fouling hydrogels are ideal vehicles for drug and cell delivery. For each application, hydrogel degradation rate must be re-optimized for maximum therapeutic benefit. We developed a method to rapidly and predictably tune degradation rates of low-fouling poly(oligo(ethylene glycol)methyl ether methacrylate) (P(EG)xMA) hydrogels by modifying two interdependent variables: (1) base-catalysed crosslink degradation kinetics, dependent on crosslinker electronics (electron withdrawing groups (EWGs)); and, (2) polymer hydration, dependent on the molecular weight (MW) of poly(ethylene glycol) (PEG) pendant groups. By controlling PEG MW and EWG strength, P(EG)xMA hydrogels were tuned to degrade over 6 to 52 d. A 6-member P(EG)xMA copolymer library yielded slow and fast degrading low-fouling hydrogels suitable for short- and long-term delivery applications. The degradation mechanism was also applied to RGD-functionalized poly(carboxybetaine methacrylamide) (PCBMAA) hydrogels to achieve slow (∼50 d) and fast (∼13 d) degrading low-fouling, bioactive hydrogels.

To tune degradation rates of low-fouling hydrogels, a 6-member P(EG)xMA copolymer library with different electronics and hydration levels was developed.
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