期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 26, 页码 9866-9871出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c03686
关键词
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资金
- BASF California Research Alliance (CARA)
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-SC0019001]
- National Science Foundation Graduate Research Fellowship
- Nippon Shokubai Ltd.
- U.S. Department of Energy (DOE) [DE-SC0019001] Funding Source: U.S. Department of Energy (DOE)
A novel grafting-through polymerization strategy was introduced to synthesize dynamic bottlebrush polymers and elastomers using light to construct a disulfide-containing backbone. The key starting material, alpha-lipoic acid (LA), is commercially available, inexpensive, and biocompatible. The resulting bottlebrush elastomers exhibit high gel fractions and tunable shear moduli, with the added benefit of dynamic disulfide bonds allowing for self-healing and on-demand chemical degradation.
We introduce a novel grafting-through polymerization strategy to synthesize dynamic bottlebrush polymers and elastomers in one step using light to construct a disulfide-containing backbone. The key starting material-alpha-lipoic acid (LA)-is commercially available, inexpensive, and biocompatible. When installed on the chain end(s) of poly(dimethylsiloxane) (PDMS), the cyclic disulfide unit derived from LA polymerizes under ultraviolet (UV) light in ambient conditions. Significantly, no additives such as initiator, solvent, or catalyst are required for efficient gelation. Formulations that include bis-LA-functionalized cross-linker yield bottlebrush elastomers with high gel fractions (83-98%) and tunable, supersoft shear moduli in the similar to 20-200 kPa range. An added advantage of these materials is the dynamic disulfide bonds along each bottlebrush backbone, which allow for light-mediated self-healing and on-demand chemical degradation. These results highlight the potential of simple and scalable synthetic routes to generate unique bottlebrush polymers and elastomers based on PDMS.
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