Unraveling the Molecular Origin of Prey-Wrapping Spider Silk's Unique Mechanical Properties and Assembly Process Using NMR

Chalek, Kevin; Onofrei, David; Aldana, Julian E.; Johnson, Hannah R.; Stengel, Dillan; Chau, Andy T.; Domingo, Anikin Rae; Alcala, Erik; Tsui, Esther; Botello, Francisco; Soni, Ashana; Addison, Bennett; Holland, Gregory P.

doi:10.1002/adfm.202409321

Title: Unraveling the Molecular Origin of Prey-Wrapping Spider Silk's Unique Mechanical Properties and Assembly Process Using NMR

Journal Article · Sat Jul 20 00:00:00 UTC 2024 · Advanced Functional Materials

DOI: https://doi.org/10.1002/adfm.202409321 · OSTI ID:2426392

Chalek, Kevin ^[1]; Onofrei, David ^[1]; Aldana, Julian E. ^[1]; Johnson, Hannah R. ^[1]; Stengel, Dillan ^[1]; Chau, Andy T. ^[1]; Domingo, Anikin Rae ^[1]; Alcala, Erik ^[1]; Tsui, Esther ^[1]; Botello, Francisco ^[1]; Soni, Ashana ^[1]; Addison, Bennett ^[2];

^[1]

San Diego State Univ., CA (United States)
National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Prey wrapping spider silk's unique mechanical properties are investigated confirming the silk's high degree of extensibility and superior toughness compared to other types of spider silk. For the first time, the pre-spinning dope phase is studied in isotope-enriched intact aciniform (AC) silk glands using solution NMR that reveals a combination of α-helical domains linked by disordered random coil chains consistent with previously proposed “beads-on-a-string” models. The model is further refined through the AlphaFold2 protein structure prediction tool. Finally, extensive magic angle spinning (MAS) solid-state (SS) NMR data for isotopically-enriched fibers is used to refine the structural model for AC silk from two species, A. aurantia and A. argentata. The SSNMR data shows that the AC silk fibers are highly α-helical, coiled-coil in structure but, also exhibit significant β-sheet components that can be traced back to the Gly-rich disordered linker regions in the pre-spinning dope phase that are converted to β-sheet structures during fiber formation. This combination of mechanical and structural characterization enhances the understanding of AC silk's liquid-to-solid transition and structure-mechanics relationship. In conclusion, these prey wrap silk results and models will provide the basis for the design of biomimetic materials inspired by the AC spider silk system.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: US Army Research Office (ARO); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 2426392

Report Number(s):: NREL/JA--2800-90558; MainId:92336; UUID:9a23a01f-5f5f-425a-9a39-f5e5021981c8; MainAdminId:73291

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 15 Vol. 35; ISSN 1616-301X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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59 BASIC BIOLOGICAL SCIENCES
nmr
nuclear magnetic resonance
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Title: Unraveling the Molecular Origin of Prey-Wrapping Spider Silk's Unique Mechanical Properties and Assembly Process Using NMR

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