Author Correction: Layered nanocomposites by shear-flow-induced alignment of nanosheets.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Layered nanocomposites by shear-flow-induced alignment of nanosheets.

Biological materials, such as bones, teeth and mollusc shells, are well known for their excellent strength, modulus and toughness1-3. Such properties are attributed to the elaborate layered microstructure of inorganic reinforcing nanofillers, especially two-dimensional nanosheets or nanoplatelets, within a ductile organic matrix4-6. Inspired by these biological structures, several assembly strategies-including layer-by-layer4,7,8, casting9,10, vacuum filtration11-13 and use of magnetic fields14,15-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.

Large-Area Layered Membranes with Precisely Controlled Nano-Confined Channels.

Two-dimensional (2D) nanosheets-based membranes, which have controlled 2D nano-confined channels, are highly desirable for molecular/ionic sieving and confined reactions. However, it is still difficult to develop an efficient method to prepare large-area membranes with high stability, high orientation, and accurately adjustable interlayer spacing. Here, we present a strategy to produce metal ion cross-linked membranes with precisely controlled 2D nano-confined channels and high stability in different solutions using superspreading shear-flow-induced assembly strategy. For example, membranes based on graphene oxide (GO) exhibit interlayer spacing ranging from 8.0±0.1 Što 10.3±0.2 Å, with a precision of down to 1 Å. At the same time, the value of the orientation order parameter (f) of GO membranes is up to 0.95 and GO membranes exhibit superb stability in different solutions. The strategy we present, which can be generalized to the preparation of 2D nano-confined channels based on a variety of 2D materials, will expand the application scope and provide better performances of membranes.

Confined Synthesis of Two-Dimensional Covalent Organic Framework Thin Films within Superspreading Water Layer.

The confined synthesis of two-dimensional covalent organic framework (2D COF) thin films was developed by using thin superspreading water on the hydrogel immersed under oil as reactor. Through loading two monomers into oil and hydrogel, respectively, COF thin films are synthesized at the oil/water/hydrogel interface. This strategy provides a new way for synthesis of freestanding 2D COF thin films. Detailed characterizations of the COF thin films reveal homogeneous topography, large area, controllable thickness from 4 to 150 nm, and crystallinity with certain orientation. Young's modulus of COF film is measured by AFM indentation as 25.9 ± 0.6 GPa, showing good mechanical properties. On the basis of the freestanding COF films, a nanofilter membrane and photoelectrochemical sensors for Ru3+ were successfully developed. Moreover, the strategy was extended to the synthesis of crystalline zeolitic imidazolate framework-8 thin film, which exhibited high application potential.

Superspreading on Immersed Gel Surfaces for the Confined Synthesis of Thin Polymer Films.

Liquid spreading is of significant interest in science and technology. Although surface topography engineering and liquid surface-tension regulating can facilitate spreading, the spreading layers in these strategies are inevitably inhomogeneous or contaminated with surfactants. Herein, we show a general strategy to realize the superspreading of liquids on mutually soluble gel surfaces. The cooperation of the hydraulic pressure under liquid phase and liquid-like property of gel surfaces can dramatically eliminate the local pinning effect and enhance the advancement of three-phase contact line, thus forming stable and homogeneous superspreading liquid layers. Such liquid layers can be converted into various functional thin polymer films with controlled thicknesses (nm- to µm-scale) through one-step polymerization of the reactants. Our strategy offers opportunities for large-scale synthesis of versatile functional thin films for various applications.

Superwetting Injectable Hydrogel with Ultrastrong and Fast Tissue Adhesion for Minimally Invasive Hemostasis.

Injectable hydrogels have recently emerged as alternatives to sutures for various clinical indications. However, existing injectable hydrogels are unsuitable for hemostasis in minimally invasive surgery because of their weak interfacial adhesion and complex/prolonged processing. Herein, a superwetting injectable hydrogel composed of oppositely charged polysaccharides is developed. The spontaneous spreading of the injectable hydrogel on the surfaces achieves complete wetting and forms tight interfacial contact by absorbing the interfacial water. The superwetting ability and subsequent covalent crosslinking perform fast and ultrastrong wet adhesion (140 kPa) on the tissue surface. Ex vivo porcine and in vivo rat models show that the hydrogel successfully leads to the aggregation of erythrocytes for targeted hemostasis (in less than 12 s) without requiring external adjuncts, and no postsurgical adhesions to the peripheral tissues. This further demonstrates that hydrogel can act as an effective hemostasis agent in laparoscopic surgery in a rabbit model. Overall, the strong wet adhesion, antibacterial properties, and easy operability make this injectable hydrogel a promising candidate for hemostasis applications, as it can successfully combine clinical efficacy and transformation opportunities for minimally invasive surgery.

Large-Area Ultrastrong and Stiff Layered MXene Nanocomposites by Shear-Flow-Induced Alignment of Nanosheets.

To shield increasingly severe radiation pollution, ultrathin MXene-based electromagnetic interference (EMI) shielding materials with excellent mechanical properties are urgently demanded in wearable electrical devices or aerospace fields. However, it is still a challenge to fabricate ultrastrong and stiff MXene-based nanocomposites with excellent EMI shielding capacity in a universal and scalable manner. Here, inspired by the natural nacre structure, we propose an efficient superspreading strategy to construct a highly oriented layered "brick-and-mortar" structure using shear-flow-induced alignment of MXene nanosheets at an immiscible hydrogel/oil interface. A continuous and large-area MXene nanocomposite film has been fabricated through a homemade industrial-scale continuous fabrication setup. The prepared MXene nanocomposite films exhibit a tensile strength of 647.6 ± 56 MPa and a Young's modulus of 59.8 ± 6.1 GPa, respectively. These outstanding mechanical properties are attributed to the continuous interphase layer that formed between the well-aligned MXene nanosheets. Moreover, the obtained MXene nanocomposites also show great EMI shielding effectiveness (51.6 dB). We consider that our MXene-based nanocomposite films may be potentially applied as electrical or aerospace devices with superior mechanical properties and high EMI shielding capacity.

Recent Advances in Bioinspired Gel Surfaces with Superwettability and Special Adhesion.

Engineering surface wettability is of great importance in academic research and practical applications. The exploration of hydrogel-based natural surfaces with superior properties has revealed new design principles of surface superwettability. Gels are composed of a cross-linked polymer network that traps numerous solvents through weak interactions. The natural fluidity of the trapped solvents confers the liquid-like property to gel surfaces, making them significantly different from solid surfaces. Bioinspired gel surfaces have shown promising applications in diverse fields. This work aims to summarize the fundamental understanding and emerging applications of bioinspired gel surfaces with superwettability and special adhesion. First, several typical hydrogel-based natural surfaces with superwettability and special adhesion are briefly introduced, followed by highlighting the unique properties and design principles of gel-based surfaces. Then, the superwettability and emerging applications of bioinspired gel surfaces, including liquid/liquid separation, antiadhesion of organisms and solids, and fabrication of thin polymer films, are presented in detail. Finally, an outlook on the future development of these novel gel surfaces is also provided.

General Strategy to Fabricate Highly Filled Microcomposite Hydrogels with High Mechanical Strength and Stiffness.

Conventional synthetic hydrogels are intrinsically soft and brittle, which severely limits the scope of their applications. A variety of approaches have been proposed to improve the mechanical strength of hydrogels. However, a facile and ubiquitous strategy to prepare hydrogels with high mechanical strength and stiffness is still a challenge. Here, we report a general strategy to prepare highly filled microcomposite hydrogels with high mechanical performance using an ultrasonic assisted strategy. The microparticles were dispersed in the polymer network evenly, resulting in homogeneous and closely packed structures. The as-prepared hydrogels with extraordinary mechanical performance can endure compressive stress up to 20 MPa (at 75% strain) and exhibit high stiffness (elastic modulus is around 18 MPa). By using our comprehensive strategy, different hydrogels can enhance their mechanical strength and stiffness by doping various microparticles, leading to a much wider variety of applications.

Covalent tethering of photo-responsive superficial layers on hydrogel surfaces for photo-controlled release.

The diffusion and transport of substances between a hydrogel and its environment have received tremendous research interest, due to the wide range of applications of hydrogel materials in fields related to drug carriers and drug delivery vehicles. To date, much research has been done to tailor the diffusion and transport of substances through hydrogels, where most efforts were focused on tuning the 3D network properties of the hydrogel including loop size, hydrophobicity of building blocks and the stimuli-responsive properties of backbones. These conventional strategies, however, usually suffer from complicated fabrication procedures and result in a homogeneous increase in hydrophobicity of the hydrogel network, leading to low efficiency control over the diffusion of substances through the hydrogel. Herein, a facile strategy that can functionalize the surfaces of hydrogels, while keeping the interior network unchanged, was reported, and is realized by quaternization reaction confined to the hydrogel/oil interface. Owing to the introduction of the photo-responsive molecule IBSP as a modifier, the surface wettability of the resulting hydrogel can be controlled by light both in air and underwater environments. Consequently, the diffusion rate of a substance through this modified hydrogel can be regulated by light, which brings convenience to the controlled release of hydrogels and other hydrogel-related fields.