Hierarchically structured bioinspired nanocomposites

Nepal, Dhriti; Kang, Saewon; Adstedt, Katarina; Kanhaiya, Krishan; Bockstaller, Michael R.; Brinson, L. Catherine; Buehler, Markus J.; Coveney, Peter V.; Dayal, Kaushik; El‐Awady, Jaafar A.; Henderson, Luke C.; Kaplan, David L.; Keten, Sinan; Kotov, Nicholas A.; Schatz, George C.; Vignolini, Silvia; Vollrath, Fritz; Wang, Yusu; Yakobson, Boris I.; Tsukruk, Vladimir V.; Heinz, Hendrik

doi:10.1038/s41563-022-01384-1

Cited by 240 publications

(150 citation statements)

References 124 publications

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“…The ability to self-repair and resume active function upon incurring structural damage is an attribute of living organisms that has inspired research to enhance material performance and sustainability. − Concepts that have been proven successful to instigate “self-healing ability” comprise the integration of vessel-type reservoirs into materials, the integration of nanofillers to enable coupling to external fields, and the use of dynamic and reversible bond networks. − While each of these concepts has shown promise, they are limited by manufacturing constraints, scalability, or cost and chemical sensitivity. An intriguing new concept for realizing self-repair capability in engineering polymers is based on copolymers with “interlocking chain architectures”. , “Interlocking” is realized by a suitable choice of copolymer compositions such that the spacing of side groups results in tooth wheel-type “interlocked” microstructures that promote dispersion interactions between the chains.…”

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Sequence-Enhanced Self-Healing in “Lock-and-Key” Copolymers

Zhao

Yin

et al. 2023

ACS Macro Lett.

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Van der Waals-driven self-healing in copolymers with “lock-and-key” architecture has emerged as a concept to endow engineering-type polymers with the capacity to recover from structural damage. Complicating the realization of “lock-and-key”-enabled self-healing is the tendency of copolymers to form nonuniform sequence distributions during polymerization reactions. This limits favorable site interactions and renders the evaluation of van der Waals-driven healing difficult. Here, methods for the synthesis of lock-and-key copolymers with prescribed sequence were used to overcome this limitation and enable the deliberate synthesis of “lock-and-key” architectures most conducive to self-healing. The effect of molecular sequence on the material’s recovery behavior was evaluated for the particular case of three poly(n-butyl acrylate/methyl methacrylate) [P(BA/MMA)] copolymers with similar molecular weights, dispersity, and overall composition but with different sequences: alternating (alt), statistical (stat), and gradient (grad). They were synthesized using atom transfer radical polymerization (ATRP). Copolymers with alt and stat sequence displayed a 10-fold increase of recovery rate compared to the grad copolymer variant despite a similar overall glass transition temperature. Investigation with small-angle neutron scattering (SANS) revealed that rapid property recovery is contingent on a uniform microstructure of copolymers in the solid state, thus avoiding the pinning of chains in glassy MMA-rich cluster regions. The results delineate strategies for the deliberate design and synthesis of engineering polymers that combine structural and thermal stability with the ability to recover from structural damage.

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confidence: 99%

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confidence: 99%

Sequence-Enhanced Self-Healing in “Lock-and-Key” Copolymers

Zhao

Yin

et al. 2023

ACS Macro Lett.

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“…The synthesis of complex, versatile, and sustainable tooth-inspired materials will benefit from computer simulations, which have already shown great advantage in understanding the structure–property relationship of biomaterials [ 105 , 106 ] and guiding the rational materials design [ 107 , 108 , 109 , 110 , 111 ]. In the future, precise manufacture will be supported by multiscale simulation techniques and data-driven approaches [ 112 , 113 ] for the highly efficient replication of diverse tooth structures with optimized functions.…”

Section: Outlook and Perspectivementioning

confidence: 99%

Tooth Diversity Underpins Future Biomimetic Replications

2023

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Although the evolution of tooth structure seems highly conserved, remarkable diversity exists among species due to different living environments and survival requirements. Along with the conservation, this diversity of evolution allows for the optimized structures and functions of teeth under various service conditions, providing valuable resources for the rational design of biomimetic materials. In this review, we survey the current knowledge about teeth from representative mammals and aquatic animals, including human teeth, herbivore and carnivore teeth, shark teeth, calcite teeth in sea urchins, magnetite teeth in chitons, and transparent teeth in dragonfish, to name a few. The highlight of tooth diversity in terms of compositions, structures, properties, and functions may stimulate further efforts in the synthesis of tooth-inspired materials with enhanced mechanical performance and broader property sets. The state-of-the-art syntheses of enamel mimetics and their properties are briefly covered. We envision that future development in this field will need to take the advantage of both conservation and diversity of teeth. Our own view on the opportunities and key challenges in this pathway is presented with a focus on the hierarchical and gradient structures, multifunctional design, and precise and scalable synthesis.

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“…Hierarchical assembly of multiple components into sophisticated structures is vital to the structural complexity and functional versatility of biological systems. − A prominent example is the hierarchical assemblies made up of DNA molecules and histone proteins, which package meter-long DNA molecules into compact structures, thus preventing the entanglement of the genetic polymers. − During the hierarchical assembly process, these histone proteins function as “anchors” that dramatically regulate the assembly pathway of DNA strands. The hierarchical structuring commonly encountered in biological materials provides inspiration for the design of synthetic materials from the bottom-up self-assembly with sophisticated functions. − Although a plethora of supramolecular systems have been programmed through self-assembly, artificial hierarchical assemblies are still limited in creating long-range ordered (orderliness repeated over great distances) superstructures from structurally dissimilar synthetic building blocks. This gap stems from the fact that biological systems are able to program the specificity of chemical interactions between structurally dissimilar components, leading to the hierarchical assembly along a given pathway. − Translating this concept to artificial assembling systems remains a grand challenge.…”

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Controlled Hierarchical Self-Assembly of Nanoparticles and Chiral Molecules into Tubular Nanocomposites

Cheng

Zhang

et al. 2023

J. Am. Chem. Soc.

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In this work, we show how the kinetics of molecular self-assembly can be coupled with the kinetics of the colloidal self-assembly of inorganic nanoparticles, which in turn drives the formation of several distinct hierarchically assembled tubular nanocomposites with lengths over tens of micrometers. These colloidal nanoparticles primarily serve as "artificial histones," around which the asassembled supramolecular fibrils are wound into deeply kinetically trapped singlelayered nanotubes, which leads to the formation of tubular nanocomposites that are resistant to supramolecular transformation thermally. Alternatively, when these nanoparticles are aggregated prior to the event of molecular self-assembly, these asformed nanoparticle "oligomers" would be encapsulated into the thermodynamically favored double-layer supramolecular nanotubes, which enables the non-closepacking of nanoparticles inside the nanotubes and results in the nanoparticle superlattices with an open channel. Furthermore, increasing the amounts of nanoparticles enables the assembly of nanoparticles into pseudohexagonal superlattices at the external surface in a sequential fashion, which ultimately drives the formation of triple-layered hierarchically assembled tubular nanocomposites. Importantly, the sense of helicity transfers from the supramolecular nanotubes to the pseudo nanoparticle superlattices with a chiral vector of (2, 9). Our findings represent a strategy for controlling the hierarchical assembly bridging supramolecular chemistry to the inorganic solids to realize the complexity by design.

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Hierarchically structured bioinspired nanocomposites

Cited by 240 publications

References 124 publications

Sequence-Enhanced Self-Healing in “Lock-and-Key” Copolymers

Sequence-Enhanced Self-Healing in “Lock-and-Key” Copolymers

Tooth Diversity Underpins Future Biomimetic Replications

Controlled Hierarchical Self-Assembly of Nanoparticles and Chiral Molecules into Tubular Nanocomposites

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