Soft Matrix Research Articles

Peptide-dendrimer-reinforced bioinks for 3D bioprinting of heterogeneous and biomimetic in vitro models.

Despite 3D bioprinting having emerged as an advanced method for fabricating complex in vitro models, developing suitable bioinks that fulfill the opposing requirements for the biofabrication window still remains challenging. Although naturally derived hydrogels can better mimic the extracellular matrix (ECM) of numerous tissues, their weak mechanical properties usually result in architecturally simple shapes and patchy functions of in vitro models. Here, this limitation is addressed by a peptide-dendrimer-reinforced bioink (HC-PDN) which contained the peptide-dendrimer branched PEG with end-grafted norbornene (PDN) and the cysteamine-modified HA (HC). The extensive introduction of ethylene end-groups facilitates the grafting of sufficient moieties and enhances thiol-ene-induced crosslinking, making HC-PDN exhibits improved mechanical and rheological properties, as well as a significant reduction in reactive oxygen species (ROS) accumulation than that of methacrylated hyaluronic acid (HAMA). In addition, HC-PDN can be applied for the bioprinting of numerous complex structures with superior shape fidelity and soft matrix microenvironment. A heterogeneous and biomimetic hepatic tissue is concretely constructed in this work. The HepG2-C3As, LX-2s, and EA.hy.926s utilized with HC-PDN and assisted GelMA bioinks closely resemble the parenchymal and non-parenchymal counterparts of the native liver. The bioprinted models show the endothelium barrier function, hepatic functions, as well as increased activity of drug-metabolizing enzymes, which are essential functions of liver tissue in vivo. All these properties make HC-PDN a promising bioink to open numerous opportunities for in vitro model biofabrication. STATEMENT OF SIGNIFICANCE: In this manuscript, we introduced a peptide dendrimer system, which belongs to the family of hyperbranched 3D nanosized macromolecules that exhibit high molecular structure regularity and various biological advantages. Specifically, norbornene-modified peptide dendrimer was grafted onto PEG, and hyaluronic acid (HA) was selected as a base material for bioink formulation because it is a component of the ECM. Peptide dendrimers confer the following advantages to bioinks: (a) Geometric symmetry can facilitate construction of bioinks with homogeneous networks; (b) abundant surface functional groups allow for abundant crosslinking points; (c) the biological origin can promote biocompatibility. This study shows conceptualization to application of a peptide-dendrimer bioink to extend the Biofabrication Window of natural bioinks and will expand use of 3D bioprinting of in vitro models.

An iteration-based interactive attention network for 3D point cloud registration

Several learning-based methods dedicated to 3D point cloud registration have been developed recently. However, the performance of such methods is limited due to a lack of effective feature interaction mechanisms. To overcome this problem, an iteration-based interactive attention network is proposed here for 3D point cloud registration that can effectively learn the overlapping features of point cloud pairs and improve the registration accuracy. Concretely, we first designed a condensed global information extractor to achieve aggregated global features. Meanwhile, to reduce the amount of calculation required for subsequent modules while maintaining high-level characteristic information, the number of point cloud features is reduced. Furthermore, an overlapping feature iterative attention module and a discriminant feature iterative expansion module are designed. The main function of both modules is to implement feature interaction in the form of cross-attention and self-attention as well as to deepen interactions iteratively. The former captures overlapping information by iteratively interacting with the features of the condensed global features of one point cloud and the local geometric features of another point cloud. The latter can expand the number of features back to the initial number of point clouds through the interaction of overlapping features and local geometric features. Finally, matching features with high discriminative ability are obtained and used to formulate a soft correspondence matrix. Furthermore, weighted singular-value decomposition is adopted to obtain the rigid transformation matrix. Extensive experiments demonstrate that the proposed method achieves state-of-the-art performance.

Soft Expert Matrix Theory and Its Application in Decision-making

Soft Expert Matrix Theory and Its Application in Decision-making

Curved adhesions mediate cell attachment to soft matrix fibres in three dimensions

Integrin-mediated focal adhesions are the primary architectures that transmit forces between the extracellular matrix (ECM) and the actin cytoskeleton. Although focal adhesions are abundant on rigid and flat substrates that support high mechanical tensions, they are sparse in soft three-dimensional (3D) environments. Here we report curvature-dependent integrin-mediated adhesions called curved adhesions. Their formation is regulated by the membrane curvatures imposed by the topography of ECM protein fibres. Curved adhesions are mediated by integrin ɑvβ5 and are molecularly distinct from focal adhesions and clathrin lattices. The molecular mechanism involves a previously unknown interaction between integrin β5 and a curvature-sensing protein, FCHo2. We find that curved adhesions are prevalent in physiological conditions, and disruption of curved adhesions inhibits the migration of some cancer cell lines in 3D fibre matrices. These findings provide a mechanism for cell anchorage to natural protein fibres and suggest that curved adhesions may serve as a potential therapeutic target.

3D Volumetric Mechanosensation of MCF7 Breast Cancer Spheroids in a Linear Stiffness Gradient GelAGE.

The tumor microenvironment presents spatiotemporal shifts in biomechanical properties with cancer progression. Hydrogel biomaterials like GelAGE offer the stiffness tuneability to recapitulate dynamic changes in tumor tissues by altering photo-energy exposures. Here, a tuneable hydrogel with spatiotemporal control of stiffness and mesh-network is developed. The volume of MCF7 spheroids encapsulated in a linear stiffness gradient demonstrates an inverse relationship with stiffness (p<0.0001). As spheroids are exposed to increased crosslinking (stiffer) and greater mechanical confinement, spheroid stiffness increases. Protein expression (TRPV4, β1 integrin, E-cadherin, and F-actin) decreases with increasing stiffness while showing strong correlations to spheroid volume (r2 >0.9). To further investigate the role of volume, MCF7 spheroids are grown in a soft matrix for 5 days prior to a second polymerisation which presents a stiffness gradient to equally expanded spheroids. Despite being exposed to variable stiffness, these spheroids show even protein expression, confirming volume as a key regulator. Overall, this work showcases the versatility of GelAGE and demonstrates volume expansion as a key regulator of 3D mechanosensation in MCF7 breast cancer spheroids. This platform has the potential to further investigation into the role of stiffness and dimensionality in 3D spheroid culture for other types of cancers and diseases.

Microstructural evolution in shear-punch tests: A comparative study of pure Cu and Cu-Cr alloy

Understanding the mechanisms behind microstructural evolution during shear deformation has been a long-standing area of interest. However, establishing a connection between microstructure, mechanical properties, and the extent of shear deformation is challenging and requires refined experimental approaches. Shear-punch testing (SPT) provides a controlled method to introduce shear into small volumes of material that later can be subjected to detailed microstructural characterization. In this study, we utilize an SPT device to induce shear deformation to pure copper (Cu) and a binary copper-chromium (Cu-Cr) alloy. Electron backscatter diffraction and transmission electron microscopy were used to study the mechanisms of plastic deformation after SPT. Our results indicate that shear deformation of pure Cu produces a dense network of intercepting microshear bands upon sustained deformation. Twin boundaries in annealed Cu undergo transformation into high-angle grain boundaries due to simultaneous deviation from the axis-angle pair condition of 60° misorientation on [111] direction. The presence of 50 vol% Cr particles in the soft Cu matrix altered the shear deformation mechanism. Preferential deformation of the Cu matrix in Cu-Cr alloy led to accelerated shear-induced formation of low and high-angle grain boundaries and subsequent grain refinement. Comparatively, insignificant grain refinement occurred in pure Cu samples even at a strain ∼10 times larger (ε = 4.73) than that of the Cu-Cr case (ε = 0.42). This study sheds light on the microstructural evolution of Cu during shear deformation and highlights the significant influence of a hard second phase in modifying the microstructural response mechanisms of a softer matrix.

In Situ Regeneration of Oxidized Copper Flakes Forming Nanosatellite Particles for Non‐Oxidized Highly Conductive Copper Nanocomposites

AbstractCopper (Cu) is an attractive low‐cost alternative to silver or gold. However, it is susceptible to oxidation in air. Here, facile in situ regeneration of oxidized Cu flakes (CuFLs) for the synthesis of highly conductive non‐oxidized nanocomposites is reported. The oxidized CuFLs are regenerated into non‐oxidized CuFLs and Cu nanosatellite (CuNS) particles by formic acid‐aided in situ etching and reduction reaction in soft epoxy matrix. The average particle size of CuNS particles is only 3.3 nm with an interparticle distance of 2.7 nm. Furthermore, the negligible potential barrier height between Cu and epoxy dramatically increases the electrical conductivity (66 893 S cm−1) of the nanocomposite (Cu = 46 vol%) by more than three orders of magnitude. The thermal conductivity is also highest (85.1 W m−1 K−1), compared with Cu‐based nanocomposites in literature. The conductivities are invariant in air for more than 95 days. The simple scalable in situ regeneration of oxidized CuFLs may find immediate industrial applications.

Constitutive formulations for intrinsic anisotropy in soft electroelastic materials

Inspired by biology and engineered soft active material systems, we propose a new constitutive formulation for a soft material consisting of soft contractile fibers embedded in a soft matrix. The mathematical implementation of the model is based on a multi-field invariant formulation within a nonlinear continuum mechanics framework. The coupled constitutive formulation highlights a new electromechanical coupling term that describes the intrinsic (or active) anisotropy due to the contractile units. The model demonstrates the relative role that intrinsic anisotropy plays in the overall stress response. The resulting formulation could be used to design and inspire the development of new soft material systems that seek to replicate three dimensional biological motion.

Modification of melt memory effect by addition of poly(butylene terephthalate) to thermoplastic polyester elastomer

The structure and properties of a thermoplastic polyester elastomer (TPEE) containing a small amount of poly(butylene terephthalate) (PBT) were investigated by focusing on the residual crystals in the molten state. When the pure TPEE was extruded at a slightly higher temperature than its melting point, the crystallization rate increased. This phenomenon has been called the melt memory effect and has been attributed to unmolten crystals that act as nuclei. The addition of PBT widened the temperature range of the melt memory effect, because PBT crystals were present at the higher temperatures. Moreover, the addition of PBT induced phase separation, leading to a decrease in the dissolution of hard segments in the soft matrix. As a result, the glass transition temperature of the soft matrix decreased. Furthermore, the modulus at room temperature increased with good rubber elasticity.

Collective Behavior of Asperities Before Large Stick‐Slip Events

AbstractThe multi‐scale roughness of a fault interface is responsible for multiple asperities that establish a complex and discrete set of real contacts. Since asperities control the initiation and evolution of the fault slip, it is important to explore the intrinsic relationships between the collective behavior of local asperities and the frictional stability of the global fault. Here we propose a novel analog experimental approach, which allows us to capture the temporal evolution of the slip of each asperity on a faulting interface. We find that many destabilizing events at the local asperity scale occurred in the slip‐strengthening stage which is conventionally considered as the stable regime of a fault. We compute the interseismic coupling to evaluate the slipping behaviors of asperities during the slip‐strengthening stage. We evidence that the interseismic coupling can be affected by the elastic interactions between asperities through the embedding soft matrix. Scaling laws of natural slow slip events are reproduced by our setup in particular the moment‐duration scaling. We also evidence an unexpected persistency of a disordering of the asperities through the seismic cycles despite the relaxation effects of the large slip events.

Enhancement of the mechanical properties and water barrier properties of thermoplastic starch nanocomposite films by chitin nanofibers: Biodegradable coating for extending banana shelf life

Starch-based films have limited applications due to their hydrophilicity and poor mechanical performance. Herein, thermoplastic starch (TPS) nanocomposite films with chitin nanofibers (ChNFs) extracted from shrimp-shell waste were successfully fabricated using a solvent casting method. We investigated the effects of the ChNF loadings on the physical, mechanical, and water vapor barrier properties of the nanocomposite films. The well-dispersed ChNFs within the soft matrix associated with the formation of interfacial bonding between ChNFs and starch facilitated the efficient stress transfer from the soft matrix to the stiff ChNFs. Additionally, the presence of ChNFs created tortuous pathways within the films, which could impede the diffusion of water molecules. This resulted in a significant improvement in the mechanical properties, wettability, water resistance, and water vapor barrier properties of the nanocomposites. Compared to the results obtained from the neat TPS films, the TPS nanocomposites reinforced with ChNFs exhibited a 300% higher tensile stress, a 603% Young's modulus, and a considerable increase in the water contact angle, shifting from 86.2° to 98.6°. Furthermore, the ChNF-reinforced nanocomposite films showed no fragmentation after being soaked in water for 12 h under vigorous stirring, whereas the neat TPS films disintegrated under the same conditions. Interestingly, we found that coating a suspension of TPS and ChNFs on bananas effectively delayed their aging, preventing the color change from green to yellow. This promising result demonstrates the potential of the developed coating to extend the shelf life of fresh food produce, reducing food waste and the reliance on single-use petroleum-based packaging.

Effect of heat treatment on microstructure and functional properties of additively manufactured NiTi shape memory alloys

Additive manufacturing of NiTi shape memory alloys has attracted attention in recent years, due to design flexibility and feasibility to achieve four-dimensional (4D) function response. To obtain customized 4D functional responses in NiTi structures, tailorable phase transformation temperatures and stress windows as well as one-way or two-way shape memory properties are required. To achieve this goal, various heat treatments, including direct aging, annealing and annealing followed by aging, were optimized for the Ti-rich NiTi (Ni49.6Ti (at. %)) fabricated by laser powder bed fusion (L-PBF). Microstructural evolution, phase transformation, precipitation and shape memory behaviour were systematically investigated by multiscale correlative microstructural, differential scanning calorimetry analysis and thermomechanical analysis. Based on optimized heat treatments, ∼25 K phase transformation temperature windows and ∼90 MPa stress windows were achieved for the one-way shape memory effect. Solutionized annealing was found to be the most effective way to improve one-way shape memory degradation resistance, due to the reduction of defects and solid solution strengthening. One of the main findings of this study is that the heterogonous microstructures between hard intergranular Ti2NiOx and soft NiTi matrix, induced by solutionized annealing with subsequent aging, result in strain partitioning and enclosing the internal stress state, which was found to promote a pronounced two-way shape memory effect response. The results of this work provide in-depth knowledge on tailoring and designing functional shape memory characteristics via heat treatments, which contributes to expanding L-PBF NiTi application fields, such as biomedical implants, aerospace components, and other advanced engineering applications.

Matrix stiffness regulates neovascular homeostasis through autophagy in nude mice.

One of the major obstacles to the effective application of vascularized fruit is an insufficient understanding of the relationship between the microenvironment and neovascular homeostasis. The role of extracellular matrixstiffness in regulating the structural and functional stability of neovascularization has not yet been elucidated. This study explored the effects of matrix stiffness on neovascular homeostasis in nude mice. Dextran hydrogels with three different stiffnesses were separately combined with mouse bone marrow-derived endothelial progenitor cells (EPCs) and subcutaneously implanted into the backs of nude mice. After 14 days, neovascular homeostasis indicators in the different groups were measured. Cell autophagy levels were evaluated, and inhibitor assays were performed to explore the underlying mechanism. New blood vessels were generated in the three stiffnesses of the EPC-loaded dextran hydrogels 14 days after implantation. The newly formed vessels tended to have better structural stability in softer hydrogels. Endothelial function markers, such as endothelial nitric oxide synthaseand E-selectin, were downregulated as the matrix stiffness increased. Furthermore, we found that cell autophagy levels decreased in stiffer matrices, and autophagy inhibition attenuated neovascular homeostasis. A soft matrix is conducive to maintaining neovascular homeostasis through autophagy in nude mice.

YAP Inactivation by Soft Mechanotransduction Relieves MAFG for Tumor Cell Dedifferentiation.

Solid tumor cells live in a highly dynamic mechanical microenvironment. How the extracellular-matrix-generated mechanotransduction regulates tumor cell development and differentiation remains an enigma. Here, we show that a low mechanical force generated from the soft matrix induces dedifferentiation of moderately stiff tumor cells to soft stem-cell-like cells. Mechanistically, integrin β8 was identified to transduce mechano-signaling to trigger tumor cell dedifferentiation by recruiting RhoGDI1 to inactivate RhoA and subsequently Yes-associated protein (YAP). YAP inactivation relieved the inhibition of v-maf avian musculoaponeurotic fibrosarcoma oncogene homolog G (MAFG), allowing MAFG to transactivate the stemness genes NANOG, SOX2, and NESTIN. Inactivation also restored β8 expression, thereby forming a closed mechanical loop. Importantly, MAFG expression is correlated with worse prognosis. Our findings provide mechanical insights into the regulation of tumor cell dedifferentiation, which has therapeutic implications for exploring innovative strategies to attack malignancies.

A Mass-In-Mass Metamaterial Design for Harvesting Energy at a Broadband Frequency Range

A novel deterministic method to harvest energy within a broadband frequency (0~25 kHz) from a mass-in-mass metamaterial is presented herein. Traditional metamaterials are composed of multiple materials (named as resonators and matrix) with different mechanical properties (e.g., stiffness, density). In this work, the stiffnesses of matrix materials are altered systematically to allow diversified property mismatches between the constituent components to introduce local resonance in the unit cell. While local resonance leverages wave energy passing through the acoustic metamaterials trapped within the relatively soft matrix as dynamic strain energy, a strategic and deterministic methodology is investigated to obtain a broadband local resonance frequency. The frequency band can then be utilized to harvest the trapped energy by embedding a smart material inside the matrix which is capable of electromechanical transduction (e.g., lead zirconate titanate). This concept has been proved numerically by harvesting energy at a broadband frequency with a power density of ~10 μW/in2. Finally, an experimental study is performed to prove the hypothesis proposed in this article.

Thermo‐mechanical property enhancement of rigid polyurethane foam composite using low cost, environment friendly fly ash over silica particles

AbstractLow cost and environment friendly fly ash particles and silica particles were used as additives in the rigid polyurethane foam composite. The usage of fly ash will decrease the need for its handling and exposure to environment. FTIR spectra show the absence of hydrogen bonded urea which indicates no aggregation of hard urea domains in the soft polyurethane matrix after the addition of silica/fly ash. The composite loaded with 20 weight percentage fly ash had the highest glass transition temperature. At 10 weight percentage of the additive, the gross calorific value in the fly ash loaded composite decreased by 12% when compared with the composite loaded with silica. Introduction of fly ash into the foam composite up to a certain weight percentage (10 wt%) enhanced the compressive strength of the rigid polyurethane foam composite. The percolate particle concentration was at 10 weight percentage of the additive. The addition of fly ash increased the compressive strength up to 21% compared to the foam composite loaded with silica. Addition of fly ash in the foam composite resulted in a decrease of water absorption up to 23% in comparison to the composite loaded with silica. Hence, low cost and environment friendly fly ash is suitable additive which can be loaded into rigid polyurethane foams for superior enhancement in mechanical and thermal properties.Highlights The addition of fly ash to the foam decreased the gross calorific value up to 12% compared to that of the silica loaded foam composite. The composite loaded with fly ash had highest normalized compressive strength and highest glass transition temperature than that of the unloaded foam. This can potentially replace conventional rigid polyurethane foam in timber constructions because of its higher compressive strength. We propose the addition of fly ash as a low cost, environment friendly additive as it improved the various properties of the polyurethane foam composite to a greater extent than silica particles. The greater usage of fly ash will help in the formation of a closed loop supply chain and alleviate the need for disposal of fly ash.

Self-Assembly of Polymer-Modified FePt Magnetic Nanoparticles and Block Copolymers.

The fabrication of nanocomposites containing magnetic nanoparticles is gaining interest as a model for application in small electronic devices. The self-assembly of block copolymers (BCPs) makes these materials ideal for use as a soft matrix to support the structural ordering of the nanoparticles. In this work, a high-molecular-weight polystyrene-b-poly(methyl methacrylate) block copolymer (PS-b-PMMA) was synthesized through anionic polymerization. The influence of the addition of different ratios of PMMA-coated FePt nanoparticles (NPs) on the self-assembled morphology was investigated using transmission electron microscopy (TEM) and small-angle X-ray scattering (SAXS). The self-assembly of the NPs inside the PMMA phase at low particle concentrations was analyzed statistically, and the negative effect of higher particle ratios on the lamellar BCP morphology became visible. The placement of the NPs inside the PMMA phase was also compared to theoretical descriptions. The magnetic addressability of the FePt nanoparticles inside the nanocomposite films was finally analyzed using bimodal magnetic force microscopy and proved the magnetic nature of the nanoparticles inside the microphase-separated BCP films.

Significant hardening effect of high-temperature aging of alloy Ti-6Al-4V composite reinforced with TiC

Titanium alloy composites, reinforced with a light second phase and made using inexpensive powder metallurgy, attract considerable attention due to the directness of their intentional hardness increase without compromising low weight of materials. In this study the metal-matrix composites (MMC) of Ti-6Al-4V alloy reinforced with light and hard particles of TiC (up to 80%, vol.) were made using blended elemental powder metallurgy of hydrogenated titanium. Post-sintering solution treatment for 45 min. at 880 °C and 1000 °C and water quenching followed by the 5 hrs. aging at 550 °C was used to additionally refine the microstructure and properties of MMC. For the duration of thermal exposure throughout solution treatment and additional aging the matrix and reinforcement phase underwent distinct structural changes that modified the mechanical properties of materials. It has been shown that the used reinforcement presents an exceptional opportunity for hardening of Ti-based composites without compromising their low specific weigh. It can increase the hardness of material by more than 40% due to the ability of TiC to chemically react with the matrix to form a strong interfacial bond and its ability to form hard compounds of Ti2C and Ti3AlC in the expense of the relatively soft matrix alloy.

A super wear-resistant coating for Mg alloys achieved by plasma electrolytic oxidation and discontinuous deposition

Magnesium alloys are lightweight materials with great potential, and plasma electrolytic oxidation (PEO) is effective surface treatment for necessary improvement of corrosion resistance of magnesium alloys. However, the ∼14 µm thick and rough PEO protection layer has inferior wear resistance, which limits magnesium alloys as sliding or reciprocating parts, where magnesium alloys have special advantages by their inherent damping and denoising properties and attractive light-weighting. Here a novel super wear-resistant coating for magnesium alloys was achieved, via the discontinuous sealing (DCS) of a 1.3 µm thick polytetrafluoroethylene (PTFE) polymer layer with an initial area fraction (Af) of 70% on the necessary PEO protection layer by selective spraying, and the wear resistance was exceptionally enhanced by ∼5500 times in comparison with the base PEO coating. The initial surface roughness (Sa) under PEO+DCS (1.54 µm) was imperfectly 59% higher than that under PEO and conventional continuous sealing (CS). Interestingly, DCS was surprisingly 20 times superior for enhancing wear resistance in contrast to CS. DCS induced nano-cracks that splitted DCS layer into multilayer nano-blocks, and DCS also provided extra space for the movement of nano-blocks, which resulted in rolling friction and nano lubrication. Further, DCS promoted mixed wear of the PTFE polymer layer and the PEO coating, and the PTFE layer (HV: 6 Kg·mm−2, Af: 92.2%) and the PEO coating (HV: 310 Kg·mm−2, Af: 7.8%) served as the soft matrix and the hard point, respectively. Moreover, the dynamic decrease of Sa by 29% during wear also contributed to the super wear resistance. The strategy of depositing a low-frictional discontinuous layer on a rough and hard layer or matrix also opens a window for achieving super wear-resistant coatings in other materials.

Fracture spacings of fiber inclusions in a ductile geological matrix and development of microboudins: 3D numerical modeling

Tensile fractures and resultant microboudinage structures of brittle fiber inclusions (e.g., tourmaline, piedmontite and amphibole) in the soft matrix of deforming minerals are of great significance for determining the finite strains and paleostresses of naturally deformed rocks. Using statistical strength theory, damage mechanics, and continuum mechanics, we have reproduced in a series of numerical models the sequential fractures of either homogeneous or heterogeneous fiber inclusions under axial tension in an elastoplastic matrix. The results clarify that: (1) The spacing between fractures in fibers is inversely proportional to the applied strain. As the applied strain increases, the fracture spacing systematically decreases as sequential fractures fill in until fracture saturation is reached. (2) As fiber length increases, the critical tensile strain for fracture saturation rises. For the same fiber diameter, saturation fracture spacing increases slightly with rising fiber length. For the same fiber length, however, saturation fracture spacing decreases significantly with lessening fiber diameter. Hence, fracture spacing at the saturation state depends on the volume fraction of fiber. (3) The rupture mode of fibers strongly depends on the non-uniform distribution of mechanical properties, which provides an effective approach for estimating the inhomogeneity of fibers by analyzing the formation of fractures. Furthermore, due to material heterogeneity, new fractures are unlikely to occur in the middle of existing adjacent fractures.