We report the preparation and structural and mechanical characterization of a tough supramolecular hydrogel, based exclusively on hydrophobic association. The system consists of a multiblock, ...segmented copolymer of hydrophilic poly(ethylene glycol) (PEG) and hydrophobic dimer fatty acid (DFA) building blocks. A series of copolymers containing 2K, 4K, and 8K PEG were prepared. Upon swelling in water, a network is formed by self-assembly of hydrophobic DFA units in micellar domains, which act as stable physical cross-link points. The resulting hydrogels are noneroding and contain 75–92 wt % of water at swelling equilibrium. Small-angle neutron scattering (SANS) measurements showed that the aggregation number of micelles ranges from 2 × 102 to 6 × 102 DFA units, increasing with PEG molecular weight. Mechanical characterization indicated that the hydrogel containing PEG 2000 is mechanically very stable and tough, possessing a tensile toughness of 4.12 MJ/m3. The high toughness, processability, and ease of preparation make these hydrogels very attractive for applications where mechanical stability and load bearing features of soft materials are required.
Nanocomposite hydrogels based on carbon nanotubes (CNTs) are known to possess remarkable stiffness, electrical, and thermal conductivity. However, they often make use of CNTs as fillers in covalently ...cross‐linked hydrogel networks or involve direct cross‐linking between CNTs and polymer chains, limiting processability properties. Herein, nanocomposite hydrogels are developed, in which CNTs are fillers in a physically cross‐linked hydrogel. Supramolecular nanocomposites are prepared at various CNT concentrations, ranging from 0.5 to 6 wt%. Incorporation of 3 wt% of CNTs leads to an increase of the material's toughness by over 80%, and it enhances electrical conductivity by 358%, compared to CNT‐free hydrogel. Meanwhile, the nanocomposite hydrogels maintain thixotropy and processability, typical of the parent hydrogel. The study also demonstrates that these materials display remarkable cytocompatibility and support cell growth and proliferation, while preserving their functional activities. These supramolecular nanocomposite hydrogels are therefore promising candidates for biomedical applications, in which both toughness and electrical conductivity are important parameters.
Supramolecular nanocomposite hydrogels are fabricated starting from a hydrophobically assembled physical gel and multi‐walled carbon nanotubes. Prepared nanocomposites are characterized by improved tensile toughness and electrical conductivity, due to dispersed nanotubes. Moreover, these supramolecular nanocomposites are fully processable and recoverable. Being also cytocompatible and able to support cell growth and proliferation, these gels are suitable for biomedical applications.
End‐stage liver diseases are an increasing health burden, and liver transplantations are currently the only curative treatment option. Due to a lack of donor livers, alternative treatments are ...urgently needed. Human liver organoids are very promising for regenerative medicine; however, organoids are currently cultured in Matrigel, which is extracted from the extracellular matrix of the Engelbreth‐Holm‐Swarm mouse sarcoma. Matrigel is poorly defined, suffers from high batch‐to‐batch variability and is of xenogeneic origin, which limits the clinical application of organoids. Here, a novel hydrogel based on polyisocyanopeptides (PIC) and laminin‐111 is described for human liver organoid cultures. PIC is a synthetic polymer that can form a hydrogel with thermosensitive properties, making it easy to handle and very attractive for clinical applications. Organoids in an optimized PIC hydrogel proliferate at rates comparable to those observed with Matrigel; proliferation rates are stiffness‐dependent, with lower stiffnesses being optimal for organoid proliferation. Moreover, organoids can be efficiently differentiated toward a hepatocyte‐like phenotype with key liver functions. This proliferation and differentiation potential maintain over at least 14 passages. The results indicate that PIC is very promising for human liver organoid culture and has the potential to be used in a variety of clinical applications including cell therapy and tissue engineering.
Liver organoids are very promising for cell therapy and tissue engineering. However, organoids are cultured in Matrigel, which limits their clinical application. Here, a novel synthetic hydrogel for human liver organoid cultures is described. Organoids efficiently proliferate and differentiate in this polyisocyanopeptides (PIC)‐based hydrogel. As such, PIC is a promising material for human liver organoid culture and enables their clinical translation.
Physically associated hydrogels based on strong hydrophobic interactions often have attractive mechanical properties that combine processability with elasticity. However, there is a need to study ...such interactions and understand their relation to the macroscopic hydrogel properties. Therefore, we use the surfactant sodium dodecyl sulfate (SDS) and urea as reagents that disrupt hydrophobic interactions. The model hydrogel is based on a segmented copolymer between poly(ethylene glycol) (PEG) and hydrophobic dimer fatty acid (DFA). We show that both agents influence viscoelastic properties, dynamics, and relaxation processes of the model hydrogel. In particular, the relaxation time is significantly reduced by urea, as compared to SDS, whereas the surfactant causes a decrease of the modulus of the hydrogel more efficiently. The reversibility of the effects of SDS and urea can be exploited, for instance, by using an injectable sol that solidifies when the SDS or urea diffuses out of the sample. Surfactant-induced processability may be advantageous in future applications of hydrophobically assembled physical hydrogels.
The load-bearing function of articular cartilage tissue contrasts with the poor load-bearing capacity of most soft hydrogels used for its regeneration. The present study explores whether a hydrogel ...based on the methacrylated natural polymers chondroitin sulfate (CSMA) and hyaluronic acid (HAMA), injected into warp-knitted spacer fabrics, could be used to create a biomimetic construct with cartilage-like mechanical properties. The swelling ratio of the combined CSMA/HAMA hydrogels in the first 20 days was higher for hydrogels with a higher CSMA concentration, and these hydrogels also degraded quicker, whereas those with a 1.33 wt% of HAMA were stable for more than 120 days. When confined by a polyamide 6 (PA6) spacer fabric, the volumetric swelling of the combined CSMA/HAMA gels (10 wt%, 6.5 × CSMA:HAMA ratio) was reduced by ~53%. Both the apparent peak and the equilibrium modulus significantly increased in the PA6-restricted constructs compared to the free-swelling hydrogels after 28 days of swelling, and no significant differences in the moduli and time constant compared to native bovine cartilage were observed. Moreover, the cell viability in the CSMA/HAMA PA6 constructs was comparable to that in gelatin–methacrylamide (GelMA) PA6 constructs at one day after polymerization. These results suggest that using a HydroSpacer construct with an extracellular matrix (ECM)-like biopolymer-based hydrogel is a promising approach for mimicking the load-bearing properties of native cartilage.
Hydrogels based on photocrosslinkable Hyaluronic Acid Methacrylate (HAMA) and Chondroitin Sulfate Methacrylate (CSMA) are presently under investigation for tissue engineering applications. HAMA and ...CSMA gels offer tunable characteristics such as tailorable mechanical properties, swelling characteristics, and enzymatic degradability. This review gives an overview of the scientific literature published regarding the pre-clinical development of covalently crosslinked hydrogels that (partially) are based on HAMA and/or CSMA. Throughout the review, recommendations for the next steps in clinical translation of hydrogels based on HAMA or CSMA are made and potential pitfalls are defined. Specifically, a myriad of different synthetic routes to obtain polymerizable hyaluronic acid and chondroitin sulfate derivatives are described. The effects of important parameters such as degree of (meth)acrylation and molecular weight of the synthesized polymers on the formed hydrogels are discussed and useful analytical techniques for their characterization are summarized. Furthermore, the characteristics of the formed hydrogels including their enzymatic degradability are discussed. Finally, a summary of several recent applications of these hydrogels in applied fields such as cartilage and cardiac regeneration and advanced tissue modelling is presented.
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LEAP: Learning Articulated Occupancy of People Mihajlovic, Marko; Zhang, Yan; Black, Michael J. ...
2021 IEEE/CVF Conference on Computer Vision and Pattern Recognition (CVPR),
2021-June
Conference Proceeding
Odprti dostop
Substantial progress has been made on modeling rigid 3D objects using deep implicit representations. Yet, extending these methods to learn neural models of human shape is still in its infancy. Human ...bodies are complex and the key challenge is to learn a representation that generalizes such that it can express body shape deformations for unseen subjects in unseen, highly-articulated, poses. To address this challenge, we introduce LEAP (LEarning Articulated occupancy of People), a novel neural occupancy representation of the human body. Given a set of bone transformations (i.e. joint locations and rotations) and a query point in space, LEAP first maps the query point to a canonical space via learned linear blend skinning (LBS) functions and then efficiently queries the occupancy value via an occupancy network that models accurate identity- and pose-dependent deformations in the canonical space. Experiments show that our canonicalized occupancy estimation with the learned LBS functions greatly improves the generalization capability of the learned occupancy representation across various human shapes and poses, outperforming existing solutions in all settings.
Viscoelastic hydrogels are gaining interest as they possess necessary requirements for bioprinting and injectability. By means of reversible, dynamic covalent bonds, it is possible to achieve ...features that recapitulate the dynamic character of the extracellular matrix. Dually cross-linked and double-network (DN) hydrogels seem to be ideal for the design of novel biomaterials and bioinks, as a wide range of properties required for mimicking advanced and complex tissues can be achieved. In this study, we investigated the fabrication of chondroitin sulfate/hyaluronic acid (CS/HA)-based DN hydrogels, in which two networks are interpenetrated and cross-linked with the dynamic covalent bonds of very different lifetimes. Namely, Diels–Alder adducts (between methylfuran and maleimide) and hydrazone bonds (between aldehyde and hydrazide) were chosen as cross-links, leading to viscoelastic hydrogels. Furthermore, we show that viscoelasticity and the dynamic character of the resulting hydrogels could be tuned by changing the composition, that is, the ratio between the two types of cross-links. Also, due to a very dynamic nature and short lifetime of hydrazone cross-links (∼800 s), the DN hydrogel is easily processable (e.g., injectable) in the first stages of gelation, allowing the material to be used in extrusion-based 3D printing. The more long-lasting and robust Diels–Alder cross-links are responsible for giving the network enhanced mechanical strength and structural stability. Being highly charged and hydrophilic, the cross-linked CS and HA enable a high swelling capacity (maximum swelling ratio ranging from 6 to 12), which upon confinement results in osmotically stiffened constructs, able to mimic the mechanical properties of cartilage tissue, with the equilibrium moduli ranging from 0.3 to 0.5 MPa. Moreover, the mesenchymal stromal cells were viable in the presence of the hydrogels, and the effect of the degradation products on the macrophages suggests their safe use for further translational applications. The DN hydrogels with dynamic covalent cross-links hold great potential for the development of novel smart and tunable viscoelastic materials to be used as biomaterial inks or bioinks in bioprinting and regenerative medicine.
COAP: Compositional Articulated Occupancy of People Mihajlovic, Marko; Saito, Shunsuke; Bansal, Aayush ...
2022 IEEE/CVF Conference on Computer Vision and Pattern Recognition (CVPR),
2022-June
Conference Proceeding
Odprti dostop
We present a novel neural implicit representation for articulated human bodies. Compared to explicit template meshes, neural implicit body representations provide an efficient mechanism for modeling ...interactions with the environment, which is essential for human motion reconstruction and synthesis in 3D scenes. However, existing neural implicit bodies suffer from either poor generalization on highly articulated poses or slow inference time. In this work, we observe that prior knowledge about the human body's shape and kinematic structure can be leveraged to improve generalization and efficiency. We decompose the full-body geometry into local body parts and employ a part-aware encoder-decoder architecture to learn neural articulated occupancy that models complex deformations locally. Our local shape encoder represents the body deformation of not only the corresponding body part but also the neighboring body parts. The decoder incorporates the geometric constraints of local body shape which significantly improves pose generalization. We demonstrate that our model is suitable for resolving self-intersections and collisions with 3D environments. Quantitative and qualitative experiments show that our method largely outperforms existing solutions in terms of both efficiency and accuracy.
Aerogels are highly porous nanostructured materials with a high specific surface area, a very low density and a low thermal conductivity. Bio-aerogels, prepared from biopolymers, have gained interest ...for biomedical applications. While most bio-aerogels are polysaccharide-based, protein-based aerogels using silk fibroin (SF) from Bombyx mori cocoons remain underexplored. Our study delved into the impact of coagulation methods on SF aerogel properties, specifically, comparing ethanol treatment (Method 1) and sodium dihydrogen phosphate (NaH 2 PO 4) (Method 2). Aerogels obtained through Method 1 exhibited a volume shrinkage of approximately 12-22 % and a density of about 0.06-0.07 g cm-3 , while those obtained via Method 2 demonstrated a more substantial volume shrinkage of approximately 60-70 % and a higher density of around 0.2 g cm-3. These differences significantly influenced the internal structure of the aerogels, manifesting distinct morphological features of the materials. Mechanical tests revealed that SF aerogels derived from Method 2 displayed superior stress resistance at 80 % strain and higher elastic recovery when compared to samples of Method 1. In conclusion, the choice in coagulation methods broadens the mechanical property and density window for this type of aerogel which offers opportunities for a wide range of biomedical applications.
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