Predictive modelling-based design and experiments for synthesis and spinning of bioinspired silk fibres

Lin, Shangchao; Ryu, Seunghwa; Tokareva, Olena; Gronau, Greta; Jacobsen, Matthew M.; Huang, Wenwen; Rizzo, Daniel J.; Li, David; Staii, Cristian; Pugno, Nicola; Wong, Joyce Y.; Kaplan, David L.; Buehler, Markus J.

doi:10.1038/ncomms7892

Cited by 121 publications

(162 citation statements)

References 47 publications

Supporting

Mentioning

160

Contrasting

Order By: Relevance

“…For example, collagen has polyproline-and glycine-rich helices, whereas silk and elastin have β-spiral [GPGXX], linker [GP(S,Y,G)], and 3 10 -helix [GGX] repeats. These repetitions are advantageous because of the intrinsic promotion of stability through the periodic recurrence of favorable interactions (4)(5)(6)(7).…”

mentioning

confidence: 99%

Molecular tandem repeat strategy for elucidating mechanical properties of high-strength proteins

Jung

Pena‐Francesch

Saadat

et al. 2016

Proc. Natl. Acad. Sci. U.S.A.

113

View full text Add to dashboard Cite

Many globular and structural proteins have repetitions in their sequences or structures. However, a clear relationship between these repeats and their contribution to the mechanical properties remains elusive. We propose a new approach for the design and production of synthetic polypeptides that comprise one or more tandem copies of a single unit with distinct amorphous and ordered regions. Our designed sequences are based on a structural protein produced in squid suction cups that has a segmented copolymer structure with amorphous and crystalline domains. We produced segmented polypeptides with varying repeat number, while keeping the lengths and compositions of the amorphous and crystalline regions fixed. We showed that mechanical properties of these synthetic proteins could be tuned by modulating their molecular weights. Specifically, the toughness and extensibility of synthetic polypeptides increase as a function of the number of tandem repeats. This result suggests that the repetitions in native squid proteins could have a genetic advantage for increased toughness and flexibility.tandem repeat | high strength | protein | thermoplastic | squid ring teeth P roteins are heteropolymers that provide a variety of building blocks for designing biological materials (1). Proteins have several advantages as natural materials: (i) their chain length, sequence, and stereochemistry can be easily controlled, (ii) the molecular structure of proteins is well-defined (e.g., secondary, tertiary, and quaternary structures), (iii) they provide a variety of functional chemistries for conjugation to other biomolecules or polymers, and (iv) they can be designed to exhibit a variety of physical properties (2). Proteins are diverse but often display substantial similarity in sequence and 3D structure. Duplication of structural units is a natural evolutionary strategy for increasing the complexity of both globular and fibrous/ structural proteins (3). For example, collagen has polyproline-and glycine-rich helices, whereas silk and elastin have β-spiral [GPGXX], linker [GP(S,Y,G)], and 3 10 -helix [GGX] repeats. These repetitions are advantageous because of the intrinsic promotion of stability through the periodic recurrence of favorable interactions (4-7).A new family of repetitive structural proteins was recently identified in the tentacles of several squid species (8, 9). Squid have teeth-like structures inside their suckers that allow the animals to grip tightly on a diverse array of objects (10). Using the tools of molecular biology and proteomics, it has been shown that these squid ring teeth (SRT) proteins have segmented semicrystalline morphology with repetitive amorphous and crystalline domains. SRT-based materials were shown to have high elastic modulus: 4-8 GPa in air and 2-4 GPa underwater below the glass transition temperature (11). However, a clear relationship between the molecular structure and the mechanical properties of this material remains elusive. This problem is complex, because SRT proteins are polydispersed i...

show abstract

mentioning

confidence: 99%

Molecular tandem repeat strategy for elucidating mechanical properties of high-strength proteins

Jung

Pena‐Francesch

Saadat

et al. 2016

Proc. Natl. Acad. Sci. U.S.A.

113

View full text Add to dashboard Cite

show abstract

“…30 The combined multiscale use of different computational techniques such as HFBM and HLSM has also proved to be successful in reproducing the macroscopic behavior of artificial nanocomposites such as gelatin-graphene oxide fibres. 31 Mesoscale models allow the design of composite materials exhibiting tailored fracture properties, drawing inspiration from mineralized biological composites.…”

Section: Applications Of Modeling Biomaterialsmentioning

confidence: 99%

Computational modeling of the mechanics of hierarchical materials

2016

Self Cite

View full text Add to dashboard Cite

Structural hierarchy coupled with material heterogeneity is often identified in natural materials, from nano-to macroscale. It combines disparate mechanical properties, such as strength and toughness, and multifunctionality, such as smart adhesion, water repellence, self-cleaning, and self-healing. These architectures can be employed in synthetic bioinspired structured materials, also adopting constituents with superior mechanical properties, such as carbon nanotubes or graphene. Advanced computational modeling is essential to understand the complex mechanisms that couple material, structural, and topological hierarchy, merging phenomena of different nature, size, and time scales. Numerical modeling also allows extensive parametric studies for the optimization of material properties and arrangement, avoiding time-consuming and complex experimental trials and providing guidance in the fabrication of novel advanced materials. Here, we review some of the most promising approaches, with a focus on the methods developed by our group.

show abstract

“…147 This colloidal structure has recently been supported by mesocopic modeling. 148 These globules would aggregate, elongate and align as the dope flows within the duct of the gland. The molecular weight and the relative size of the hydrophobic block as compared to the hydrophilic one affect the size and structure of the globules as well as the assembly process.…”

Section: Molecular Transformations During Spinningmentioning

confidence: 99%

“…As a matter of fact, the high molecular weight of natural proteins is viewed as an important determinant to match the tensile property of the natural fibers. 148,191,192 Native-sized recombinant spidroins have recently been successfully expressed. 193,194 Interestingly, synthetic fibers made with these proteins could achieved mechanical properties close to those of the native fiber.…”

Section: Synthetic Silk Spinning Processesmentioning

confidence: 99%

“…Computer simulations now allows mesoscale approaches 309 and the study of the conversion of the spidroin molecules in solution into a fiber. 148 Still, new experimental and modelisation breakthroughs are required to fully understand the complexity and subtleties of the relation between sequence, structure and properties. To fully take advantage of silk and widen our range of models, it would also be very useful to deepen our understanding of the other types of silk, in particular those that do not possess a modular sequence pattern such as Ac silk.…”

Section: Conclusion and Future Challengesmentioning

confidence: 99%

See 1 more Smart Citation

Spider silk as a blueprint for greener materials: a review

Lefèvre

Auger

2016

International Materials Reviews

View full text Add to dashboard Cite

Spider silk exhibits remarkable properties, especially its well-known tensile performances. They rely on a complex nanostructured hierarchical organization that researches progressively elucidate. Spider silk encompasses a vast range of fibers that exhibit diverse and captivating physical and biological characteristics. The full understanding of the relation between structure and properties may lead in the future to the design of a variety of high-performance, tailored materials and devices. Reknown for being produced in mild and begnin conditions, this outstanding biological material constitutes one the more representative example of biomimetism. In addition, silk's structure is produced with limited means, i.e. low energy and relatively simple renewable constituents (silk proteins). Then, if successfully controlled and adequately transposed in biomaterials, some properties of natural silk could lead to innovative green materials that may contribute to reduce the ecological footprint of societies. In fact, striking recent advanced applications made with B. mori silk suggest that spider silk-based materials may lead to advanced resistant and functional materials, then becoming among the most promising subject of study in material science. However, several challenges have to be overcome, especially our ability to produce native-like silk, to control biomaterials' structure and properties, and to minimize their ecological footprint. This paper reviews the characteristics of spider silk that make it so attractive and that may (or may not) contribute to reduce ecological footprint of materials and the challenges in producing innovative spider silk-based materials. First, from a biomimetic perspective, the structure and models that explain the tensile resistance of natural silk are presented, followed by the state of knowledge regarding natural silk spinning process and synthetic production methods. Biocompatibility (biosafety and biofunctionality) as well as biodegradability issues are then addressed. Finally, examples of applications are reviewed. Features that may lead to the design of green materials are emphasized throughout.

show abstract

Predictive modelling-based design and experiments for synthesis and spinning of bioinspired silk fibres

Cited by 121 publications

References 47 publications

Molecular tandem repeat strategy for elucidating mechanical properties of high-strength proteins

Molecular tandem repeat strategy for elucidating mechanical properties of high-strength proteins

Computational modeling of the mechanics of hierarchical materials

Spider silk as a blueprint for greener materials: a review

Contact Info

Product

Resources

About