Abstract:
:The mechanical properties of Bombyx mori silk fibroin (SF), such as elasticity and tensile strength, change remarkably upon hydration. However, the microscopic interaction with water is not currently well understood on a molecular level. In this work, the dynamics of water molecules interacting with SF was studied by 2H solution NMR relaxation and exchange measurements. Additionally, the conformations of hydrated [3-13C]Ala-, [3-13C]Ser-, and [3-13C]Tyr-SF fibers and films were investigated by 13C DD/MAS NMR. Using an inverse Laplace transform algorithm, we were able to identify four distinct components in the relaxation times for water in SF fiber. Namely, A: bulk water outside the fiber, B: water molecules trapped weakly on the surface of the fiber, C: bound water molecules located in the inner surface of the fiber, and D: bound water molecules located in the inner part of the fiber were distinguishable. In addition, four components were also observed for water in the SF film immersed in methanol for 30s, while only two components for the film immersed in methanol for 24h. The effects of hydration on the conformation of Ser and Tyr residues in the site-specific crystalline and non-crystalline domains of 13C selectively labeled SF, respectively, could be determined independently. Our measurements provide new insight relating the characteristics of water and the hydration structure of silk, which are relevant in light of current interest in the design of novel silk-based biomaterials. STATEMENTS OF SIGNIFICANCE:The mechanical properties of Bombyx mori silk fibroin (SF) change remarkably upon hydration. However, the microscopic interaction between SF and water is not currently well understood on a molecular level. We were able to identify four distinct components in the relaxation times for water in SF fiber by 2H solution NMR relaxation and exchange measurements. In addition, the effects of hydration on the conformation of Ser and Tyr residues in the site-specific crystalline and non-crystalline domains of 13C selectively labeled SF, respectively, could be determined independently. Thus, our measurements provide new insight relating the characteristics of water and the hydration structure of silk, which are relevant in light of current interest in the design of novel silk-based biomaterials.
journal_name
Acta Biomaterjournal_title
Acta biomaterialiaauthors
Asakura T,Isobe K,Kametani S,Ukpebor OT,Silverstein MC,Boutis GSdoi
10.1016/j.actbio.2016.12.052subject
Has Abstractpub_date
2017-03-01 00:00:00pages
322-333eissn
1742-7061issn
1878-7568pii
S1742-7061(16)30733-4journal_volume
50pub_type
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