期刊
ADVANCED FUNCTIONAL MATERIALS
卷 23, 期 9, 页码 1111-1119出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.201201922
关键词
biomimetics; hydrogels; polymeric materials; structure-property relationships
类别
资金
- MRSEC program of the National Science Foundation at the Northwestern University Materials Research Science and Engineering Center [DMR-1121262]
- NIH
- IBNAM-Baxter Early Career Development Award in Bioengineering [F30HL096292]
- NIH National Research Service Award from the National Heart, Lung, and Blood Institute [F30HL096292]
- Danish Council for Independent Research, Natural Sciences [272-08-0087]
- University of Chicago Materials Research Science and Engineering Center [DMR 0820054]
- NSF [MCB-0920316]
- Direct For Biological Sciences
- Div Of Molecular and Cellular Bioscience [0920316] Funding Source: National Science Foundation
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [820054] Funding Source: National Science Foundation
The mechanical holdfast of the mussel, the byssus, is processed at acidic pH yet functions at alkaline pH. Byssi are enriched in Fe3+ and catechol-containing proteins, species with chemical interactions that vary widely over the pH range of byssal processing. Currently, the link between pH, Fe3+-catechol reactions, and mechanical function is poorly understood. Herein, it is described how pH influences the mechanical performance of materials formed by reacting synthetic catechol polymers with Fe3+. Processing Fe3+-catechol polymer materials through a mussel-mimetic acidic-to-alkaline pH change leads to mechanically tough materials based on a covalent network fortified by sacrificial Fe3+-catechol coordination bonds. These findings offer the first direct evidence of Fe3+-induced covalent cross-linking of catechol polymers, reveal additional insight into the pH dependence and mechanical role of Fe3+-catechol interactions in mussel byssi, and illustrate the wide range of physical properties accessible in synthetic materials through mimicry of mussel-protein chemistry and processing.
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