期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 19, 页码 22271-22281出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c06178
关键词
inflammatory response; nonsteroidal anti-inflammatory drug; shape memory; thermal healing; polylactic acid; bone tissue engineering
资金
- BRIDGE award from the University of Massachusetts Medical School
- National Institutes of Health [R01AR055615, R01GM088678]
By copolymerizing aspirin-functionalized glycolide with D,L-lactide, this study successfully enhanced the thermal processing, toughness, and shape-memory efficiency of PLA-based implants while mitigating degradation-induced chronic inflammation. The inclusion of aspirin pendants in the copolymers significantly improved mechanical properties and shape-memory performance, making them a promising option for biomedical applications.
Synergistically modulating mechanical properties and improving shape-memory performance while mitigating degradation-induced chronic inflammation of polylactide (PLA)based implants for biomedical applications remain elusive. We test the hypothesis that copolymerizing aspirin-functionalized glycolide with D,L-lactide could enhance the thermal processing, toughness, and shape-memory efficiency of the copolymer while mitigating local inflammatory responses upon its degradation. The content of pendant aspirin was readily modulated by monomer feeds during ring-opening polymerization, and the copolymers with similar to 10% or less aspirin pendants exhibited gigapascal-tensile moduli at body temperature and significantly improved fracture toughness and energy dissipation that positively correlated with the aspirin pendant content. The copolymers also exhibited excellent thermalhealing and shape-memory efficacy, achieving a >97% temporary shape fixing ratio at room temperature and facile shape recovery at 50-65 degrees C. These drastic improvements were attributed to the dynamic hydrophobic aggregations among aspirin pendants that strengthen glassy-state physical entanglement of PLA while readily dissociating under stress/thermal activation. When subcutaneously implanted, the copolymers mitigated degradation-induced inflammation due to concomitant hydrolytic release of aspirin without suppressing early acute inflammatory responses. The incorporation of aspirin pendants in PLA represents a straightforward and innovative strategy to enhance the toughness, shape-memory performance, and in vivo safety of this important class of thermoplastics for biomedical applications.
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