Showing papers in "Soft Matter in 2019"
TL;DR: This review describes several methods commonly used for the fabrication of robust peptide-based hydrogels, including spontaneous hydrogelation, enzyme-controlled hydrogalation and cross-linking-enhanced hydrogELation, and introduces some representative studies on their applications in drug delivery and antitumor therapy, antimicrobial and wound healing materials, and 3D biop printing and tissue engineering.
Abstract: Peptide-based hydrogels have been proven to be preeminent biomedical materials due to their high water content, tunable mechanical stability, great biocompatibility and excellent injectability. The ability of peptide-based hydrogels to provide extracellular matrix-mimicking environments opens up opportunities for their biomedical applications in fields such as drug delivery, tissue engineering, and wound healing. In this review, we first describe several methods commonly used for the fabrication of robust peptide-based hydrogels, including spontaneous hydrogelation, enzyme-controlled hydrogelation and cross-linking-enhanced hydrogelation. We then introduce some representative studies on their applications in drug delivery and antitumor therapy, antimicrobial and wound healing materials, and 3D bioprinting and tissue engineering. We hope that this review facilitates the advances of hydrogels in biomedical applications.
247 citations
TL;DR: The progress and trends in marine anti-biofouling are reviewed, the mechanism and systems of DSA are presented, and coatings with dynamic surfaces by using degradable polymers are developed.
Abstract: Marine biofouling is a global problem today. High efficiency and eco-friendly antifouling systems are in pressing need. In recent years, we have proposed the concept of dynamic surface antifouling (DSA). That is, a continuously changing surface can effectively prevent marine fouling organisms from landing and adhesion. Based on this strategy, we developed coatings with dynamic surfaces by using degradable polymers including polyester-polyurethane, modified polyester and poly(ester-co-acrylate). They exhibit tunable renewability, and excellent antifouling and mechanical performance. Moreover, the polymers can serve as carrier and controlled release systems of antifoulants so that they have long service life. This paper reviews the progress and trends in marine anti-biofouling, and presents the mechanism and systems of DSA.
157 citations
TL;DR: It is concluded that-consistent with the original study-diffusion of tracers in the mucin gels is most non-Gaussian and non-ergodic at low pH that corresponds to the most heterogeneous networks.
Abstract: Native mucus is polymer-based soft-matter material of paramount biological importance. How non-Gaussian and non-ergodic is the diffusive spreading of pathogens in mucus? We study the passive, thermally driven motion of micron-sized tracers in hydrogels of mucins, the main polymeric component of mucus. We report the results of the Bayesian analysis for ranking several diffusion models for a set of tracer trajectories [C. E. Wagner et al., Biomacromolecules, 2017, 18, 3654]. The models with “diffusing diffusivity”, fractional and standard Brownian motion are used. The likelihood functions and evidences of each model are computed, ranking the significance of each model for individual traces. We find that viscoelastic anomalous diffusion is often most probable, followed by Brownian motion, while the model with a diffusing diffusion coefficient is only realised rarely. Our analysis also clarifies the distribution of time-averaged displacements, correlations of scaling exponents and diffusion coefficients, and the degree of non-Gaussianity of displacements at varying pH levels. Weak ergodicity breaking is also quantified. We conclude that—consistent with the original study—diffusion of tracers in the mucin gels is most non-Gaussian and non-ergodic at low pH that corresponds to the most heterogeneous networks. Using the Bayesian approach with the nested-sampling algorithm, together with the quantitative analysis of multiple statistical measures, we report new insights into possible physical mechanisms of diffusion in mucin gels.
139 citations
TL;DR: The rheological and adhesive properties of PVP-TA coacervate hydrogels are analyzed, revealing that they could exhibit not only a self-healing property, but also super adhesive properties with an average adhesion strength of 3.71 MPa on a glass substrate, which is >4 times stronger than that of conventional PVP.
Abstract: When multiple intermolecular interactions occur simultaneously, complexed molecules undergo gelation by inter-cohesive bonding, inducing a pseudo-crosslinking effect to form a supramolecular gel. Among the number of substances that can induce supramolecular assembly, phenolic species such as 3,4-dihydroxy-L-phenylalanine (DOPA) are widely utilized for synthesizing adhesive materials. However, despite the strong adhesion capability of monomeric phenol, it lacks cohesive strength and rarely forms a supramolecular gel to secure its mechanical properties. In this study, to overcome this obstacle, we synthesized a supramolecular coacervate hydrogel by simply mixing poly(N-vinylpyrrolidone) (PVP) and tannic acid (TA), resulting in strong cohesive interactions by virtue of the larger molecular size of TA and reinforced molecular interactions attributed to the presence of galloyl groups with a high density. We further analyzed the rheological and adhesive properties of PVP–TA coacervate hydrogels, revealing that they could exhibit not only a self-healing property, but also super adhesive properties with an average adhesion strength of 3.71 MPa on a glass substrate, which is >4 times stronger than that of conventional PVP.
104 citations
TL;DR: The results demonstrated that the prepared supramolecular hydrogels possessed different mechanisms in the adsorption of the four typical poisonous organic dye molecules used, including bisphenol A (BPA), 4-aminoazobenzene (N-Azo), methylene blue (MB), and rhodamine B (RhB).
Abstract: Self-assembled hydrogel materials constructed from cyclodextrin polymer (P-CD)/adamantane-modified poly acrylic acid (PAA-Ad) were designed and prepared via host-guest interactions. It was observed that the prepared supramolecular hydrogels had an interconnected three-dimensional porous network. In addition, the obtained hydrogels showed a recovery performance and it was confirmed that the host-guest interactions between β-cyclodextrin and adamantane were the main driving force for the formation of the hydrogels. The mechanical properties of the hydrogels could be adjusted by varying the concentrations of PAA-Ad. In particular, the prepared supramolecular hydrogels exhibited superior performances in water purification. The results demonstrated that the hydrogels possessed different mechanisms in the adsorption of the four typical poisonous organic dye molecules used, including bisphenol A (BPA), 4-aminoazobenzene (N-Azo), methylene blue (MB), and rhodamine B (RhB). The hydrogels mainly adsorbed N-Azo by host-guest interaction and adsorbed BPA by host-guest interaction and hydrogen bond synergy. They also adsorbed MB and RhB by hydrogen bonding and electrostatic interaction.
102 citations
TL;DR: A new and accurate method to determine the Poisson's ratio of PDMS, using thermal expansion and an optical surface profilometer, found that for both PDMS types, the coefficient of thermal expansion depends approximately linearly on the curing temperature.
Abstract: We present a new and accurate method to determine the Poisson's ratio of PDMS, using thermal expansion and an optical surface profilometer. The Poisson's ratio of Sylgard 184 was found to be ν = 0.4950 ± 0.0010 and for Sylgard 182, ν = 0.4974 ± 0.0006. Furthermore, we found that for both PDMS types, the coefficient of thermal expansion depends approximately linearly on the curing temperature. This method can be used for almost any kind of soft polymer that can be cured from a liquid at elevated temperatures.
101 citations
TL;DR: This work provides an in-depth rheological study of GO suspensions with a wide range of behaviours from Newtonian-like to viscoelastic 'printable' soft solids, and demonstrates that the quantification of 'printability' can be based on three rheology parameters.
Abstract: Additive manufacturing (AM) techniques and so-called 2D materials have undergone an explosive growth in the past decade. The former opens multiple possibilities in the manufacturing of multifunctional complex structures, and the latter on a wide range of applications from energy to water purification. Extrusion-based 3D printing, also known as Direct Ink Writing (DIW), robocasting, and often simply 3D printing, provides a unique approach to introduce advanced and high-added-value materials with limited availability into lab-scale manufacturing. On the other hand, 2D colloids of graphene oxide (GO) exhibit a fascinating rheology and can aid the processing of different materials to develop ‘printable’ formulations. This work provides an in-depth rheological study of GO suspensions with a wide range of behaviours from Newtonian-like to viscoelastic ‘printable’ soft solids. The combination of extensional and shear rheology reveals the network formation process as GO concentration increases from <0.1 vol% to 3 vol%. Our results also demonstrate that the quantification of ‘printability’ can be based on three rheology parameters: the stiffness of the network via the storage modulus (G′), the solid-to-liquid transition or flow stress (σf), and the flow transition index, which relates the flow and yield stresses (FTI = σf/σy).
97 citations
TL;DR: This perspective reports the latest ER materials along with their rheological understanding and provides a forward-looking summary of the potential future applications of ER technology.
Abstract: The characteristics of an electrorheological (ER) fluid, as a class of smart soft matter, can be actively and accurately tuned between a liquid- and a solid-like phase by the application of an electric field. ER materials used in ER fluids are electrically polarizable particles, which are attracting considerable attention in addition to further research. This perspective reports the latest ER materials along with their rheological understanding and provides a forward-looking summary of the potential future applications of ER technology.
94 citations
TL;DR: Numerical models of neutral microgels are reviewed, going from the atomistic to the single-particle level, and the state-of-the-art is described.
Abstract: Microgels are complex macromolecules. These colloid-sized polymer networks possess internal degrees of freedom and, depending on the polymer(s) they are made of, can acquire a responsiveness to variations of the environment (temperature, pH, salt concentration, etc.). Besides being valuable for many practical applications, microgels are also extremely important to tackle fundamental physics problems. As a result, these last years have seen a rapid development of protocols for the synthesis of microgels, and more and more research has been devoted to the investigation of their bulk properties. However, from a numerical standpoint the picture is more fragmented, as the inherently multi-scale nature of microgels, whose bulk behaviour crucially depends on the microscopic details, cannot be handled at a single level of coarse-graining. Here we present an overview of the methods and models that have been proposed to describe non-ionic microgels at different length-scales, from the atomistic to the single-particle level. We especially focus on monomer-resolved models, as these have the right level of details to capture the most important properties of microgels, responsiveness and softness. We suggest that these microscopic descriptions, if realistic enough, can be employed as starting points to develop the more coarse-grained representations required to investigate the behaviour of bulk suspensions.
84 citations
TL;DR: A simple yet robust magnetically actuated, aphid-inspired design of an elastomeric surface that provides rapidly tunable and highly reversible adhesion strength is reported.
Abstract: Tunable and reversible dry adhesion has attracted much attention in academia and industry due to its wide applications ranging from releasable joints to stamps for transfer printing. Here, a simple yet robust magnetically actuated, aphid-inspired design of an elastomeric surface that provides rapidly tunable and highly reversible adhesion strength is reported. The magnetically actuated adhesive features open reservoirs filled with magnetic particles and encapsulated by a thin surface membrane, which can be deformed in a controlled manner via the magnetic field, thus, to tune the adhesion. The combination of the rate dependent effect and magnetic actuation of the thin surface membrane offers continuously tunable adhesion with a great switchability and a quick response. Experimental and theoretical studies reveal the underlying physics and provide design guidelines to optimize geometries for the broad control of adhesion. Demonstrations of this concept in stamps for transfer printing of silicon wafers in air and in a vacuum with a selective and programmable mode illustrate the capabilities for deterministic assembly and the potential in the semiconductor industry.
81 citations
TL;DR: A straightforward method to directly program complex, reversible, non-planar shape changes in nematic LCEs using mechanical deformations that impart low or high strains in the LCE including stamping, curling, stretching and embossing methods is demonstrated.
Abstract: Liquid crystal elastomers (LCEs) are shape morphing materials promising for many applications including soft robotics, actuators, and biomedical devices, but current LCE synthesis techniques lack a simple method to program new and arbitrary shape changes. Here, we demonstrate a straightforward method to directly program complex, reversible, non-planar shape changes in nematic LCEs. We utilize a double network synthesis process that results in a competitive double network LCE. By optimizing the crosslink densities of the first and second network we can mechanically program non-planar shapes with strains between 4-100%. This enables us to directly program LCEs using mechanical deformations that impart low or high strains in the LCE including stamping, curling, stretching and embossing methods. The resulting LCEs reversibly shape-shift between the initial and programmed shape. This work widens the potential application of LCEs in biomedical devices, soft-robotics and micro-fluidics where arbitrary and easily programmed shapes are needed.
TL;DR: This Review follows the structure of the chains as grafting density increases, and how this structure slows relaxation of polymer chains and affects macroscopic material properties.
Abstract: Grafting polymers to nanoparticle surfaces influences properties from the conformation of the polymer chains to the dispersion and assembly of nanoparticles within a polymeric material. Recently, a small body of work has begun to address the question of how grafting polymers to a nanoparticle surface impacts chain dynamics, and the resulting physical properties of a material. This Review discusses recent work that characterizes the structure and dynamics of polymers that are grafted to nanoparticles and opportunities for future research. Starting from the case of a single polymer chain attached to a nanoparticle core, this Review follows the structure of the chains as grafting density increases, and how this structure slows relaxation of polymer chains and affects macroscopic material properties.
TL;DR: A brief overview of the physics of phase separation and its biological implications, with a particular focus on the assembly of membraneless organelles, can be found in this paper.
Abstract: The sustenance of life depends on the high degree of organization that prevails through different levels of living organisms, from subcellular structures such as biomolecular complexes and organelles to tissues and organs. The physical origin of such organization is not fully understood, and even though it is clear that cells and organisms cannot maintain their integrity without consuming energy, there is growing evidence that individual assembly processes can be thermodynamically driven and occur spontaneously due to changes in thermodynamic variables such as intermolecular interactions and concentration. Understanding the phase separation in vivo requires a multidisciplinary approach, integrating the theory and physics of phase separation with experimental and computational techniques. This paper aims at providing a brief overview of the physics of phase separation and its biological implications, with a particular focus on the assembly of membraneless organelles. We discuss the underlying physical principles of phase separation from its thermodynamics to its kinetics. We also overview the wide range of methods utilized for experimental verification and characterization of phase separation of membraneless organelles, as well as the utility of molecular simulations rooted in thermodynamics and statistical physics in understanding the governing principles of thermodynamically driven biological self-assembly processes.
TL;DR: This paper combined photopolymerization reaction kinetics and Euler-Bernoulli beam theory to study UV post-curing induced shape distortion of thin structures prepared by DLP 3D printing.
Abstract: Digital light processing (DLP) three-dimensional (3D) printing technology has advantages of fast printing speed and high printing precision. It can print objects with small and complex geometrical features and has been widely used in jewelry manufacturing and dentistry. In DLP printing, it is common to use post-treatment with UV light irradiation to improve the final mechanical properties. However, it was found that the UV post-curing process can lead to shape distortion and thus reduction of dimension accuracy. In this paper, we combined photopolymerization reaction kinetics and Euler-Bernoulli beam theory to study UV post-curing induced shape distortion of thin structures prepared by DLP 3D printing. Experiments were conducted to characterize the evolution of mechanical behavior of printed samples during the post-printing process, which was correlated to printing parameters (printing time of single-layer, height of single-layer and printing UV intensity), post-curing UV light intensity and the thickness of the strip. Moreover, post-curing induced distortion was used for the fabrication of 3D structures.
TL;DR: The syntheses and characterisation of the first ten homologues of the 1-cyanobiphenyl-4'-yl)-6-(4-alkylanilinebenzylidene-4-oxy)hexanes (CB6O.m) series showed an enantiotropic nematic, N, phase, and a monotropic twist-bend nematics, NTB, phase.
Abstract: The syntheses and characterisation of the first ten homologues of the 1-(4-cyanobiphenyl-4′-yl)-6-(4-alkylanilinebenzylidene-4′-oxy)hexanes (CB6O.m) are reported. All ten members of the series exhibit an enantiotropic nematic, N, phase, and a monotropic twist-bend nematic, NTB, phase. Only CB6O.10 shows a smectic phase. The assignment of both nematic phases was confirmed using X-ray diffraction. For short chain lengths (m = 1–6) the local packing in both nematic phases is an intercalated arrangement, for intermediate chain lengths a frustrated local structure is seen and for the longest chain length, a bilayer arrangement is observed. This change in the local structure on increasing m has no apparent effect on the stability of either nematic phase, and TNTBN and TNI show a regular dependence on m. Specifically, TNTBN and TNI decrease on increasing m and superimposed upon this is a weak odd–even effect in which the odd members show the higher values. TNI decreases more rapidly than TNTBN on increasing m such that the ratio TNTBN/TNI increases. The lower temperature liquid crystal phase shown by 1-(4-cyanobiphenyl-4′-yloxy)-5-(4-butylanilinebenzylidene-4′-oxy)pentane (CBO5O.4) is reassigned as a twist-bend nematic phase. The transitional properties of the CB6O.m, CB6O.Om and CBO5O.m series are compared.
TL;DR: This work describes a new approach for engineering cell-laden networks of aligned type I collagen fibers using 3D microextrusion printing of a collagen-Matrigel ink and demonstrates hierarchical control of 3D-printed collagen with the ability to spatially pattern collagen fiber alignment and geometry.
Abstract: Type I collagen self-assembles into three-dimensional (3D) fibrous networks. These dynamic viscoelastic materials can be remodeled in response to mechanical and chemical signals to form anisotropic networks, the structure of which influences tissue development, homeostasis, and disease progression. Conventional approaches for fabricating anisotropic networks of type I collagen are often limited to unidirectional fiber alignment over small areas. Here, we describe a new approach for engineering cell-laden networks of aligned type I collagen fibers using 3D microextrusion printing of a collagen-Matrigel ink. We demonstrate hierarchical control of 3D-printed collagen with the ability to spatially pattern collagen fiber alignment and geometry. Our data suggest that collagen alignment results from a combination of molecular crowding in the ink and shear and extensional flows present during 3D printing. We demonstrate that human breast cancer cells cultured on 3D-printed collagen constructs orient along the direction of collagen fiber alignment. We also demonstrate the ability to simultaneously bioprint epithelial cell clusters and control the alignment and geometry of collagen fibers surrounding cells in the bioink. The resulting cell-laden constructs consist of epithelial cell clusters fully embedded in aligned networks of collagen fibers. Such 3D-printed constructs can be used for studies of developmental biology, tissue engineering, and regenerative medicine.
TL;DR: The state of the art regarding simulations of ionization equilibria of weak polyelectrolytes solutions and gels is recapitulates and gaps and open problems in the existing simulation literature are identified, and challenges for future development are proposed.
Abstract: This article recapitulates the state of the art regarding simulations of ionization equilibria of weak polyelectrolyte solutions and gels. We start out by reviewing the essential thermodynamics of ionization and show how the weak polyelectrolyte ionization differs from the ionization of simple weak acids and bases. Next, we describe simulation methods for ionization reactions, focusing on two methods: the constant-pH ensemble and the reaction ensemble. After discussing the advantages and limitations of both methods, we review the existing simulation literature. We discuss coarse-grained simulations of weak polyelectrolytes with respect to ionization equilibria, conformational properties, and the effects of salt, both in good and poor solvent conditions. This is followed by a discussion of branched star-like weak polyelectrolytes and weak polyelectrolyte gels. At the end we touch upon the interactions of weak polyelectrolytes with other polymers, surfaces, nanoparticles and proteins. Although proteins are an important class of weak polyelectrolytes, we explicitly exclude simulations of protein ionization equilibria, unless they involve protein-polyelectrolyte interactions. Finally, we try to identify gaps and open problems in the existing simulation literature, and propose challenges for future development.
TL;DR: A perspective on reconstruction of cell mechanical equilibrium by reconstitution of cortical actomyosin networks in lipid membrane vesicles adhered on compliant substrates is provided and future perspectives of this active research area are discussed.
Abstract: The cytoskeleton of a cell controls all the aspects of cell shape changes and motility from its physiological functions for survival to reproduction to death. The structure and dynamics of the cytoskeletal components: actin, microtubules, intermediate filaments, and septins – recently regarded as the fourth member of the cytoskeleton family – are conserved during evolution. Such conserved and effective control over the mechanics of the cell makes the cytoskeletal components great candidates for in vitro reconstitution and bottom-up synthetic biology studies. Here, we review the recent efforts in reconstitution of the cytoskeleton in and on membrane-enclosed biomimetic systems and argue that co-reconstitution and synergistic interplay between cytoskeletal filaments might be indispensable for efficient mechanical functionality of active minimal cells. Further, mechanical equilibrium in adherent eukaryotic cells is achieved by the formation of integrin-based focal contacts with extracellular matrix (ECM) and the transmission of stresses generated by actomyosin contraction to ECM. Therefore, a minimal mimic of such balance of forces and quasi-static kinetics of the cell by bottom-up reconstitution requires a careful construction of contractile machineries and their link with adhesive contacts. In this review, in addition to cytoskeletal crosstalk, we provide a perspective on reconstruction of cell mechanical equilibrium by reconstitution of cortical actomyosin networks in lipid membrane vesicles adhered on compliant substrates and also discuss future perspectives of this active research area.
TL;DR: The authors' results show that membrane charge increases the bending rigidity relative to the charge-free membrane, and this effect is diminished by the addition of monovalent salt to the suspending solutions.
Abstract: We experimentally investigate the effect of lipid charge on the stiffness of bilayer membranes The bending rigidity of membranes with composition 0-100 mol% of charged lipids, in the absence and presence of salt at different concentrations, is measured with the flicker spectroscopy method, using the shape fluctuations of giant unilamellar vesicles The analysis considers both the mean squared amplitudes and the time autocorrelations of the shape modes Our results show that membrane charge increases the bending rigidity relative to the charge-free membrane The effect is diminished by the addition of monovalent salt to the suspending solutions The trend shown by the membrane bending rigidity correlates with zeta potential measurements, confirming charge screening at different salt concentrations The experimental results in the presence of salt are in good agreement with existing theories of membrane stiffening by surface charge
TL;DR: In this paper, the number of coexisting phases and their compositions of N-component mixtures with N > 3 was determined by constructing complete phase diagrams based on numerical convexification of the discretized free energy landscape.
Abstract: Multicomponent systems are ubiquitous in nature and industry. While the physics of few-component liquid mixtures (i.e., binary and ternary ones) is well-understood and routinely taught in undergraduate courses, the thermodynamic and kinetic properties of N-component mixtures with N > 3 have remained relatively unexplored. An example of such a mixture is provided by the intracellular fluid, in which protein-rich droplets phase separate into distinct membraneless organelles. In this work, we investigate equilibrium phase behavior and morphology of N-component liquid mixtures within the Flory-Huggins theory of regular solutions. In order to determine the number of coexisting phases and their compositions, we developed a new algorithm for constructing complete phase diagrams, based on numerical convexification of the discretized free energy landscape. Together with a Cahn-Hilliard approach for kinetics, we employ this method to study mixtures with N = 4 and 5 components. We report on both the coarsening behavior of such systems, as well as the resulting morphologies in three spatial dimensions. We discuss how the number of coexisting phases and their compositions can be extracted with Principal Component Analysis (PCA) and K-means clustering algorithms. Finally, we discuss how one can reverse engineer the interaction parameters and volume fractions of components in order to achieve a range of desired packing structures, such as nested "Russian dolls" and encapsulated Janus droplets.
TL;DR: In this perspective, why it is important to study active matter in fluids with finite inertia is focused on and interesting collective behavior to emerge is expected.
Abstract: Living matter, such as biological tissue, can be viewed as a nonequilibrium hierarchical assembly, where at each scale self-driven components come together by consuming energy in order to form increasingly complex structures. The remarkable properties of living or “active-matter” systems, as they are generally known, such as versatility, self-healing, and self-replicating, have prompted the following questions: (1) do we understand the biology and biophysics that give rise to these properties? (2) can we achieve similar functionality with synthetic active materials? In this perspective we specifically focus on why it is important to study active matter in fluids with finite inertia. Finite inertia is relevant for mesoscale organisms that swim or fly covering at least three orders of magnitude in size (≈0.5 mm–50 cm) and their collective behavior is generally unknown. As a result, we are limited both in our understanding of the biology of mesoscale swarms and processes but also in our design of self-powered machines and robots at those scales. We expect interesting collective behavior to emerge because with finite inertia, come nonlinearities and the many-body hydrodynamic interactions between the organisms/particles can become quite complex, potentially leading to phenomena, such as novel flocking states and nonequilibrium phase transitions that have not been observed before and which could have great impact in materials applications.
TL;DR: The effects that a variation of the morphology and surface chemistry of a particle can have on its ability to adhere to a liquid interface, from a thermodynamic as well as a kinetic perspective, are explored.
Abstract: The adsorption of colloidal particles to fluid interfaces is a phenomenon that is of interest to multiple disciplines across the physical and biological sciences. In this review we provide an entry level discussion of our current understanding on the physical principles involved and experimental observations of the adsorption of a single isolated particle to a liquid-liquid interface. We explore the effects that a variation of the morphology and surface chemistry of a particle can have on its ability to adhere to a liquid interface, from a thermodynamic as well as a kinetic perspective, and the impact of adsorption behaviour on potential applications. Finally, we discuss recent developments in the measurement of the interfacial behaviour of nanoparticles and highlight open questions for future research.
TL;DR: This paper systematically evaluates errors in contact angle goniometry both theoretically and experimentally, focusing on the importance of image resolution.
Abstract: The most widely used method to quantify the wetting properties of surfaces is by measuring contact angles. Even though contact angle goniometry is a powerful technique for characterizing wetting properties, it is not accurate for very hydrophobic surfaces. As the technique relies on image processing, it has inherent errors due to optical limitations, especially near the three-phase contact line. This leads to uncertainties in the positioning of the baseline, which can cause large errors in the measured contact angles. In this paper, we systematically evaluate these errors both theoretically and experimentally, focusing on the importance of image resolution. For ∼9 microliter droplet, displacement of the baseline by a single pixel leads to errors of approximately ±0.5° to ±1° for contact angles up to 150°, and errors increase rapidly in the superhydrophobic regime, up to ±8°. The error in the contact angle can be slightly reduced by increasing the image resolution, but cannot be eliminated entirely.
TL;DR: Preliminary in vitro biocompatibility and cell adhesion assays performed on Chinese hamster ovarian (CHO) cells suggest a potential employment of these multicomponent hydrogels as exogenous scaffold materials for tissue engineering.
Abstract: Short peptides or single amino acids are interesting building blocks for fabrication of hydrogels, frequently used as extracellular matrix-mimicking scaffolds for cell growth in tissue engineering. The combination of two or more peptide hydrogelators could allow obtaining different materials exhibiting new architectures, tunable mechanical properties, high stability and improved biofunctionality. Here we report on the synthesis, formulation and multi-scale characterization of peptide-based mixed hydrogels formed by the low molecular weight Fmoc-FF (Nα-fluorenylmethyloxycarbonyl diphenylalanine) hydrogelator and of the PEG8-(FY)3 hexapeptide, containing three repetitions of the Phe-Tyr motif and a PEG moiety at its N-terminus. Mixed hydrogels were also prepared by replacing PEG8-(FY)3 with its analogue (FY)3, without the PEG moiety. Rheology analysis confirmed the improved mechanical features of the multicomponent gels prepared at two different ratios (2/1 or 1/1, v/v). However, the presence of the hydrophilic PEG polymeric moiety causes a slowing down of the gel kinetic formation (from 42 to 18 minutes) and a decrease of the gel rigidity (G′ from 9 to 6 kPa). Preliminary in vitro biocompatibility and cell adhesion assays performed on Chinese hamster ovarian (CHO) cells suggest a potential employment of these multicomponent hydrogels as exogenous scaffold materials for tissue engineering.
TL;DR: A simple and economical phase separation method for fabricating superhydrophobic films using polylactic acid (PLA), nano-SiO2 and a mixture of good and poor solvents to construct a rough surface with a nano/microstructured morphology is proposed.
Abstract: Superhydrophobic films that are simple, inexpensive, corrosion-resistant and multifunctional are in high demand for industrial applications. We propose a simple and economical phase separation method for fabricating superhydrophobic films using polylactic acid (PLA), nano-SiO2 and a mixture of good and poor solvents to construct a rough surface with a nano/microstructured morphology. The phase separation-induced superhydrophobic PLA/SiO2 composite film with a porous network structure has a water contact angle greater than 164°. This method can be applied to a variety of surfaces or used in large-scale industrial production. The fabricated superhydrophobic films may be applied in biological fields because PLA is a good biodegradable material.
TL;DR: It was demonstrated that the Poisson's ratio of cellulose aerogels is not equal to zero, contrary to what is usually reported in the literature, but decreases with an increase in density.
Abstract: Highly porous and lightweight cellulose materials were prepared via dissolution–coagulation and different drying routes. Cellulose of three different molecular weights was dissolved in an ionic liquid/dimethyl sulfoxide mixture. Drying was performed either with supercritical CO2 resulting in “aerogels”, or via freeze-drying resulting in “cryogels”. The influence of cellulose molecular weight, concentration and drying method on the morphology, density, porosity and specific surface area was determined. The mechanical properties of cellulose cryogels and aerogels under uniaxial compression were studied in detail and analyzed in the view of existing models developed for porous materials. It was demonstrated that the Poisson's ratio of cellulose aerogels is not equal to zero, contrary to what is usually reported in the literature, but decreases with an increase in density. Compressive modulus and yield stress of cryogels turned out to be higher than those of aerogels taken at the same density. This was interpreted by the different morphology of the porous materials studied.
TL;DR: This work analyzes nonlinear bending deformation of a soft electret structure and examines the precise conditions that may lead to a strong emergent piezoelectric response under bending, showing that non-uniformly distributed dipoles and charges in the soft electrets lead to an apparent electromechanical response that may be ambiguously and interchangeably interpreted as either transverse piezOElectricity or flexoelectrics.
Abstract: Soft materials that exhibit electromechanical coupling are an important element in the development of soft robotics, flexible and stretchable electronics, energy harvesters, sensor and actuators. Truly soft natural piezoelectrics essentially do not exist and typical dielectric elastomers, predicated on electrostriction and the Maxwell stress effect, exhibit only a one-way electromechanical coupling. Extensive research however has shown that soft electrets i.e. materials with embedded immobile charges and dipoles, can be artificially engineered to exhibit a rather large piezoelectric-like effect. Unfortunately, this piezoelectric effect—large as it may be—is primarily restricted to an electromechanical coupling in the longitudinal direction or what is referred colloquially as the d33 piezoelectric coefficient. In sharp contrast, the transverse piezoelectric property (the so-called d31 coefficient) is rather small. This distinction has profound implications since these soft electrets exhibit negligible electromechanical coupling under bending deformation. As a result, the typically engineered soft electrets are rendered substantively ill-suited for energy harvesting as well as actuation/sensing of flexure motion that plays a critical role in applications like soft robotics. In this work, we analyze nonlinear bending deformation of a soft electret structure and examine the precise conditions that may lead to a strong emergent piezoelectric response under bending. Furthermore, we show that non-uniformly distributed dipoles and charges in the soft electrets lead to an apparent electromechanical response that may be ambiguously and interchangeably interpreted as either transverse piezoelectricity or flexoelectricity. We suggest pragmatic routes to engineer a large transverse piezoelectric (d31) and flexoelectric coefficient in soft electrets. Finally, we show that in an appropriately designed soft electret, even a uniform external electric field can induce curvature in the structure thus enabling its application as a bending actuator.
TL;DR: The co-assembly of a cell adhesive peptide conjugate (Pept-1) and alginate (ALG) is reported, to confer supramolecular hydrogels with excellent mechanical properties and high efficacy in both hemostatic control and wound healing requiring no additional growth factors.
Abstract: Injectable hydrogels are promising materials for applications in non-compressive wound management. Yet difficulties remain for the fabrication of mechanically stable hydrogel materials with inherent functionalities in both hemostatic control and wound healing without additional supplements of growth factors. Herein, we reported the co-assembly of a cell adhesive peptide conjugate (Pept-1) and alginate (ALG), to confer supramolecular hydrogels with excellent mechanical properties and high efficacy in both hemostatic control and wound healing requiring no additional growth factors. The co-assembling process of Pept-1 and ALG, which was mediated by electrostatic interactions and metal chelation, afforded a composite hydrogel with denser nanofibrillar structures and better mechanical strength when comparing to the Pept-1 gel alone. As-prepared Pept-1/ALG hydrogels exhibited excellent injectability and thixotropic properties, making them ideal materials for wound dressing. The composite hydrogel induced fast hemostasis when spiked with whole blood in vitro, and reduced the amount of bleeding to ∼18% of the untreated control in a liver puncture mouse model. Meanwhile, it promoted adhesion and migration of fibroblast NIH3T3 cells in vitro, and accelerated the rate of wound healing in a full-thickness skin defect model of mice. In addition, the Pept-1/ALG hydrogel showed excellent biocompatibility with no obvious hemolytic activity. In future, the strategy of utilizing co-assembled nanostructures composed of biofunctional peptides and polysaccharides could be further exploited to construct a broad range of nanocomposite materials for a variety of biomedical applications.
TL;DR: In this paper, the dynamics of a tunable 2D active nematic liquid crystal composed of microtubules and kinesin motors confined to an oil-water interface was studied.
Abstract: We study the dynamics of a tunable 2D active nematic liquid crystal composed of microtubules and kinesin motors confined to an oil–water interface. Kinesin motors continuously inject mechanical energy into the system through ATP hydrolysis, powering the relative microscopic sliding of adjacent microtubules, which in turn generates macroscale autonomous flows and chaotic dynamics. We use particle image velocimetry to quantify two-dimensional flows of active nematics and extract their statistical properties. In agreement with the hydrodynamic theory, we find that the vortex areas comprising the chaotic flows are exponentially distributed, which allows us to extract the characteristic system length scale. We probe the dependence of this length scale on the ATP concentration, which is the experimental knob that tunes the magnitude of the active stress. Our data suggest a possible mapping between the ATP concentration and the active stress that is based on the Michaelis–Menten kinetics that governs the motion of individual kinesin motors.
TL;DR: The enhanced adsorption of proteins onto the colloid surface significantly altered the NP identity and severely impaired the colloidal integrity as the lipophilic cargo was continuously leached out of the hydrophobic NP core.
Abstract: The majority of effort in the area of polymeric nanocarriers is aimed at providing controlled drug delivery in vivo. Therefore, it is essential to understand the delicate interplay of polymeric NPs with serum proteins in order to forecast their performance in a biological system. In this study, the interaction of serum proteins with functionalized polymeric colloids as a function of particle charge and hydrophobicity was investigated. Moreover, impact on NP stability and cargo leaching was assessed. The hard protein corona of polymeric NPs with either uncharged methoxy groups (methoxy-NPs), positively charged amine groups (amine-NPs), negatively charged carboxylic acid groups (carboxyl-NPs) or zwitterionic NPs decorated with amine and carboxylic acid groups (zwitterion-NPs) was quantitatively and qualitatively analyzed and correlated with the respective colloidal stability using fluorescence resonance energy transfer. Positively charged amine-NPs displayed an enhanced interaction with serum proteins via electrostatic interactions resulting in a hard corona consisting of diverse protein components. As revealed by FRET and agarose gel electrophoresis, the enhanced adsorption of proteins onto the colloidal surface significantly altered the NP identity and severely impaired the colloidal integrity as the lipophilic cargo was continuously leached out of the hydrophobic NP core. These results highlight the importance of generating a profound knowledge of the bio-nano interface as adherence of biomolecules can severely compromise the performance of a colloidal drug delivery system by changing its identity and integrity.