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Layered nanocomposites by shear-flow-induced alignment of nanosheets 期刊论文
NATURE, 2020, 580 (7802) : 210-+
作者:  Rollie, Clare;  Chevallereau, Anne;  Watson, Bridget N. J.;  Chyou, Te-yuan;  Fradet, Olivier;  McLeod, Isobel;  Fineran, Peter C.;  Brown, Chris M.;  Gandon, Sylvain;  Westra, Edze R.
收藏  |  浏览/下载:42/0  |  提交时间:2020/07/03

Layered nanocomposites fabricated using a continuous and scalable process achieve properties exceeding those of natural nacre, the result of stiffened matrix polymer chains confined between highly aligned nanosheets.


Biological materials, such as bones, teeth and mollusc shells, are well known for their excellent strength, modulus and toughness(1-3). Such properties are attributed to the elaborate layered microstructure of inorganic reinforcing nanofillers, especially two-dimensional nanosheets or nanoplatelets, within a ductile organic matrix(4-6). Inspired by these biological structures, several assembly strategies-including layer-by-layer(4,7,8), casting(9,10), vacuum filtration(11-13) and use of magnetic fields(14,15)-have been used to develop layered nanocomposites. However, how to produce ultrastrong layered nanocomposites in a universal, viable and scalable manner remains an open issue. Here we present a strategy to produce nanocomposites with highly ordered layered structures using shear-flow-induced alignment of two-dimensional nanosheets at an immiscible hydrogel/oil interface. For example, nanocomposites based on nanosheets of graphene oxide and clay exhibit a tensile strength of up to 1,215 +/- 80 megapascals and a Young'  s modulus of 198.8 +/- 6.5 gigapascals, which are 9.0 and 2.8 times higher, respectively, than those of natural nacre (mother of pearl). When nanosheets of clay are used, the toughness of the resulting nanocomposite can reach 36.7 +/- 3.0 megajoules per cubic metre, which is 20.4 times higher than that of natural nacre  meanwhile, the tensile strength is 1,195 +/- 60 megapascals. Quantitative analysis indicates that the well aligned nanosheets form a critical interphase, and this results in the observed mechanical properties. We consider that our strategy, which could be readily extended to align a variety of two-dimensional nanofillers, could be applied to a wide range of structural composites and lead to the development of high-performance composites.


  
Constructing protein polyhedra via orthogonal chemical interactions 期刊论文
NATURE, 2020, 578 (7793) : 172-+
作者:  Mooley, K. P.;  Deller, A. T.;  Gottlieb, O.;  Nakar, E.;  Hallinan, G.;  Bourke, S.;  Frail, D. A.;  Horesh, A.;  Corsi, A.;  Hotokezaka, K.
收藏  |  浏览/下载:8/0  |  提交时间:2020/07/03

Many proteins exist naturally as symmetrical homooligomers or homopolymers(1). The emergent structural and functional properties of such protein assemblies have inspired extensive efforts in biomolecular design(2-5). As synthesized by ribosomes, proteins are inherently asymmetric. Thus, they must acquire multiple surface patches that selectively associate to generate the different symmetry elements needed to form higher-order architectures(1,6)-a daunting task for protein design. Here we address this problem using an inorganic chemical approach, whereby multiple modes of protein-protein interactions and symmetry are simultaneously achieved by selective, '  one-pot'  coordination of soft and hard metal ions. We show that a monomeric protein (protomer) appropriately modified with biologically inspired hydroxamate groups and zinc-binding motifs assembles through concurrent Fe3+ and Zn2+ coordination into discrete dodecameric and hexameric cages. Our cages closely resemble natural polyhedral protein architectures(7,8) and are, to our knowledge, unique among designed systems(9-13) in that they possess tightly packed shells devoid of large apertures. At the same time, they can assemble and disassemble in response to diverse stimuli, owing to their heterobimetallic construction on minimal interprotein-bonding footprints. With stoichiometries ranging from [2 Fe:9 Zn:6 protomers] to [8 Fe:21 Zn:12 protomers], these protein cages represent some of the compositionally most complex protein assemblies-or inorganic coordination complexes-obtained by design.


An inorganic chemical approach to biomolecular design is used to generate '  cages'  that can simultaneously promote symmetry and multiple modes of protein interactions.


  
Design and synthesis of multigrain nanocrystals via geometric misfit strain 期刊论文
NATURE, 2020, 577 (7790) : 359-+
作者:  Oh, Myoung Hwan;  Cho, Min Gee;  Chung, Dong Young;  Park, Inchul;  Kwon, Youngwook Paul;  Ophus, Colin;  Kim, Dokyoon;  Kim, Min Gyu;  Jeong, Beomgyun;  Gu, X. Wendy;  Jo, Jinwoung;  Yoo, Ji Mun;  Hong, Jaeyoung;  McMains, Sara;  Kang, Kisuk;  Sung, Yung-Eun;  Alivisatos, A. Paul;  Hyeon, Taeghwan
收藏  |  浏览/下载:12/0  |  提交时间:2020/07/03

The impact of topological defects associated with grain boundaries (GB defects) on the electrical, optical, magnetic, mechanical and chemical properties of nanocrystalline materials(1,2) is well known. However, elucidating this influence experimentally is difficult because grains typically exhibit a large range of sizes, shapes and random relative orientations(3-5). Here we demonstrate that precise control of the heteroepitaxy of colloidal polyhedral nanocrystals enables ordered grain growth and can thereby produce material samples with uniform GB defects. We illustrate our approach with a multigrain nanocrystal comprising a Co3O4 nanocube core that carries a Mn3O4 shell on each facet. The individual shells are symmetry-related interconnected grains(6), and the large geometric misfit between adjacent tetragonal Mn3O4 grains results in tilt boundaries at the sharp edges of the Co3O4 nanocube core that join via disclinations. We identify four design principles that govern the production of these highly ordered multigrain nanostructures. First, the shape of the substrate nanocrystal must guide the crystallographic orientation of the overgrowth phase(7). Second, the size of the substrate must be smaller than the characteristic distance between the dislocations. Third, the incompatible symmetry between the overgrowth phase and the substrate increases the geometric misfit strain between the grains. Fourth, for GB formation under near-equilibrium conditions, the surface energy of the shell needs to be balanced by the increasing elastic energy through ligand passivation(8-10). With these principles, we can produce a range of multigrain nanocrystals containing distinct GB defects.


  
Form and function of F-actin during biomineralization revealed from live experiments on foraminifera 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2019, 116 (10) : 4111-4116
作者:  Tyszka, Jaroslaw;  Bickmeyer, Ulf;  Raitzsch, Markus;  Bijma, Jelle;  Kaczmarek, Karina;  Mewes, Antje;  Topa, Pawel;  Janse, Max
收藏  |  浏览/下载:9/0  |  提交时间:2019/11/27
morphogenesis  biomineralization  shells  foraminifera  cytoskeleton