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Results for “responsive hydrogels”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Computational design of microscopic swimmers and capsules: From directed motion to collective behavior

Systems of motile microscopic particles can exhibit behaviors that resemble those of living microorganisms, including cooperative motion, self-organization, and adaptability to changing environments. Using mesoscale computational modeling, we design synthetic microswimmers and microcapsules that undergo controllable, self-propelled motion in solution. Stimuli-responsive hydrogels are used to actuate the microswimmers and to enable their navigation and chemotaxing behavior. The self-propelled motion of microcapsules on solid surfaces is achieved by the release of encapsulated solutes that alter the surface adhesiveness. These signaling solutes also enable interactions among multiple microcapsules that lead to complex, cooperative behavior. Our findings provide guidelines for creating microscopic devices and machines able to autonomously move and mimic the communication and chemotaxis of biological microorganisms.

42 ENGINEERING↗
DOE OSTI2024

Material assembly from collective action of shape-changing polymers

Some animals form transient, responsive and solid-like ensembles through dynamic structural interactions. These ensembles demonstrate emergent responses such as spontaneous self-assembly, which are difficult to achieve in synthetic soft matter. In this work, we use shape-morphing units comprising responsive polymers to create solids that self-assemble, modulate their volume and disassemble on demand. The ensemble is composed of a responsive hydrogel, liquid crystal elastomer or semicrystalline polymer ribbons that reversibly bend or twist. The dispersions of these ribbons mechanically interlock, inducing reversible aggregation. The aggregated liquid crystal elastomer ribbons have a 12-fold increase in the yield stress compared with cooled dispersion and contract by 34% on heating. Ribbon type, concentration and shape dictate the aggregation and govern the global mechanical properties of the solid that forms. Coating liquid crystal elastomer ribbons with a liquid metal begets photoresponsive and electrically conductive aggregates, whereas seeding cells on hydrogel ribbons enables self-assembling three-dimensional scaffolds, providing a versatile platform for the design of dynamic materials.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Polymers with controlled assembly and rigidity made with click-functional peptide bundles

The engineering of biological molecules is a key concept in the design of highly functional, sophisticated soft materials. Biomolecules exhibit a wide range of functions and structures, including chemical recognition (of enzyme substrates or adhesive ligands, for example), exquisite nanostructures (composed of peptides, proteins or nucleic acids), and unusual mechanical properties (such as silk-like strength, stiffness, viscoelasticity and resiliency). Here we combine the computational design of physical (noncovalent) interactions with pathway-dependent, hierarchical ‘click’ covalent assembly to produce hybrid synthetic peptide-based polymers. The nanometre-scale monomeric units of these polymers are homotetrameric, α-helical bundles of low-molecular-weight peptides. These bundled monomers, or ‘bundlemers’, can be designed to provide complete control of the stability, size and spatial display of chemical functionalities. The protein-like structure of the bundle allows precise positioning of covalent linkages between the ends of distinct bundlemers, resulting in polymers with interesting and controllable physical characteristics, such as rigid rods, semiflexible or kinked chains, and thermally responsive hydrogel networks. Chain stiffness can be controlled by varying only the linkage. Moreover, by controlling the amino acid sequence along the bundlemer periphery, we use specific amino acid side chains, including non-natural ‘click’ chemistry functionalities, to conjugate moieties into a desired pattern, enabling the creation of a wide variety of hybrid nanomaterials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Correlating structural changes in thermoresponsive hydrogels to the optical response of embedded plasmonic nanoparticles

Stimuli-responsive microgels, composed of small beads with soft, deformable polymer networks swollen through a combination of synthetic control over the polymer and its interaction with water, form a versatile platform for development of multifunctional and biocompatible sensors. The interfacial structural variation of such materials at a nanometer length scale is essential to their function, but not yet fully comprehended. Here, we take advantage of the plasmonic response of a gold nanorod embedded in a thermoresponsive microgel (AuNR@PNIPMAm) to monitor structural changes in the hydrogel directly near the nanorod surface. By direct comparison of the plasmon response against measurements of the hydrogel structure from dynamic light scattering and nuclear magnetic resonance, we find that the microgel shell of batch-polymerized AuNR@PNIPMAm exhibits a heterogeneous volume phase transition reflected by different onset temperatures for changes in the hydrodyanmic radius (R H ) and plasmon resonance, respectively. The new approach of contrasting plasmonic response (a measure of local surface hydrogel structure) with R H and relaxation times paves a new path to gain valuable insight for the design of plasmonic sensors based on stimuli-responsive hydrogels.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

3D-printed ketoenamine crosslinked polyrotaxane hydrogels and their mechanochromic responsiveness

A ketoenamine-based dynamic covalent crosslinker was introduced here to α-cyclodextrin-based polypseudorotaxanes, forming viscoelastic hydrogels for direct-ink-write 3D printing. The irreversible enol–keto tautomerization imparts high chemical stability to the extensively crosslinked polyrotaxane hydrogels, which showed mechanochromic responsiveness in the presence of the integrated fluorophores.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Mussel-Inspired Hydrogel Composite with Multi-Stimuli Responsive Behavior

A mussel-inspired adhesive hydrogel with pH, temperature, and near-infrared (NIR) light–responsive behavior is designed here. The hydrogel system is formulated by combining chitosan modified with catechol motifs, thermo-responsive poly(N-isopropylacrylamide) terminated with catechols, and light-absorbing polypyrrole nanoparticles (PpyNPs). The effects of catechol concentration, molar ratio of Fe 3+ to catechol units, pH, and the incorporation of the PpyNPs on the mechanical property of the formed hydrogel are investigated. The responsive behaviors of the resulting hydrogel composite to pH, temperature, and NIR light are also demonstrated. The obtained hydrogel also shows promising adhesive property to glass and steel substrates. It is anticipated that the fabricated adhesive hydrogel with multi-responsive behavior, especially NIR light response, can potentially be useful in a wide range of biomedical applications, such as remotely controlled release systems and removable sealant materials.

42 ENGINEERING↗
DOE OSTI2015

Oxygen reduction reaction induced pH-responsive chemo-mechanical hydrogel actuators

We describe and characterize elementary designs for electrochemical micro- and macro-scale chemomechanical hydrogel actuators. The actuation of a pH-sensitive cross-linked polyacrylic acid (PAA) hydrogel is driven in the model devices through the oxygen reduction reaction (ORR) occurring at the electrodes of an embedded Au mesh micro-electrochemical array. Proton consumption by the ORR at the cathode of the embedded electrochemical cell leads to the formation of a localized pH gradient that in turn drives the strain response in the composite actuators. The dynamics result from the ionization of the carboxylic acid moieties of the PAA network in the high pH region, yielding an osmotic pressure that drives a volumetric expansion due to water imbibition. This system actuates both stably and reversibly; when the electrochemically-induced ORR is halted, the localized pH gradient dissipates due to diffusive mixing, which in turn relaxes the induced strains. Two approaches to the fabrication of hydrogel actuators were examined in this work. The first method adopted a design based on small flagella (~0.2 mm × 1.5 mm × 60 μm, width × length × height) in which the actuating PAA structures are molded atop a set of fixed electrodes mounted on a supporting substrate. These hydrogel actuators show fast, large-amplitude, and largely reversible responses in the ORR mediated chemomechanical dynamics. We also investigated larger hydrogel actuators (~4.5 mm × 11 mm × 1 mm, width × length × height), based on an autonomous design that embeds an open mesh stretchable micro-electrode array within the hydrogel. Furthermore, the significant and design-dependent impacts of mass transfer on the chemomechanical dynamics are evidenced in each case, a feature examined to elucidate more efficient mesoscopic design rules for actuators of this form.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Preparation of pH ‐responsive cellulose nanofibril/sodium alginate based hydrogels for drug release

Abstract In this work, hydrogels composed of cellulose nanofibril (CNF) and sodium alginate (SA) were prepared as a pH‐responsive release system by controlling the amount of CNF and SA. Scanning electron microscopy, thermogravimetric analysis, and swelling rate methods were used to characterize. The results showed that when the mass ratio of CNF to SA was 2:1, CNF/SA hydrogels with better morphology were obtained. Due to the deprotonation or protonation of calcium alginate, as the pH changing from 1.5 to 11.0, the swelling ratio increased from 7 times to 19 times compared with its dry weight. The drug release behaviors of the CNF/SA hydrogels using ibuprofen (IBU) as a model drug were investigated in vitro. The release of IBU was faster in alkaline conditions and slower in acidic conditions. The drug release mechanism under pH stimulation could be interpreted by the Fickian diffusion and erosion effect based on Korsmeyer‐Peppas model.

Li, Yuhang↗
DOE OSTI2021

Chemically controlled pattern formation in self-oscillating elastic shells

Significance Mechanochemical processes drive various biological functions including morphogenesis and morphological changes in responsive synthetic hydrogels. By allowing reactive components to function in an elastic closed shell, autonomous chemical reactions generate microcompartments capable of expanding or contracting or induce buckled patterns. This capability can drive specific functions such as enhancing the rate of diffusion of compartmentalized chemicals or releasing cargos at specific rates. Here, we demonstrate the coupling of mechanical response to autonomous chemical reactions in elastic shells which swell and deswell to generate specific dynamic patterns and morphologies. The reverse feedback from the mechanical input triggers the chemical reaction. Our work inspires the design of responsive shells to enhance the functionality of microcompartments and nanoreactors.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Imaging of Hydrogel Microsphere Structure and Foreign Body Response Based on Endogenous X-Ray Phase Contrast

Transplantation of functional islets encapsulated in stable biomaterials has the potential to cure Type I diabetes. However, the success of these materials requires the ability to understand their stability in vivo. Imaging techniques that enable monitoring of biomaterial performance are critical to further development in the field. In this study, we demonstrate for the first time that X-ray phase contrast (XPC) imaging techniques enable 3D imaging and evaluation of islet volume, alginate hydrogel structure and local soft tissue response. Islets were encapsulated in alginate systems prepared in methods used in clinical trials and implanted in a rodent omentum pouch model as a treatment for type I diabetes. Microbeads were imaged with XPC prior to implantation and following implantation into an omentum pouch. Islets could be identified within alginate beads and the islet volume quantified. Omental adipose tissue could be distinguished from inflammatory regions resulting from implanted beads. Individual beads and the local encapsulation response were visualized and quantifiable. Measurements were in agreement with histology. The 3D structure of the microbeads could be characterized with XPC and failed beads could also be identified. These results point to the substantial potential of XPC as a tool for imaging biomaterials in small animal models.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2019

Designing CO 2 -Responsive Multifunctional Nanoscale Fluids with Tunable Hydrogel Behavior for Subsurface Energy Recovery

The ability to direct subsurface fluid flow or achieve a high level of control on permeability in subsurface environments necessitates the development of tunable novel subsurface fluids. These multifunctional fluids should have the potential to form hydrogels to divert flow or enhance fracture networks at elevated pressures, ability to transport proppants, undergo reversible transformations from gel-like to fluid-like in response to chemical- or pressure-based perturbations, and have improved CO 2 carrying capacity for enhancing the miscibility and flowability of oil and gas. In this paper, we discuss the development of multifunctional nanofluids constructed from silica (SiO 2 ) nanoparticles and poly(allylamine) (PAA), amine bearing polymer chains with high affinity for CO 2 . A 2-fold increase in CO 2 absorption in SiO 2 -PAA nanofluids compared to the pure polymer was noted. Upon CO 2 absorption, the weakly interacting polymeric chains around the nanoparticles formed relatively compact hydrogels. Time-resolved ultrasmall-angle X-ray scattering/small-angle X-ray scattering measurements showed the transition from swollen branched polymers to Gaussian coils with an increased exposure to CO 2 . Further, CO 2 -induced hydrogel formation in aqueous fluids bearing 1 wt % SiO 2 -PAA nanofluids occurred at room temperature, unlike in fluids bearing 1 wt % PAA. These observations point to the feasibility of forming hydrogels at lower temperatures and pressures using novel nanofluids as opposed to using the pure polymer. As a result, the ability to tune the structures and morphologies of these fluids expands the potential applications of these fluids in a wide range of subsurface environments.

03 NATURAL GAS↗
DOE OSTI2025

Chemo‐Mechanical Coupling in Hydrogels: Dynamics in the Diffusion‐Limited Regime

Hydrogels are characterized by substantial volume changes in response to external stimuli, making them promising candidates for developing smart materials with enhanced adaptability and responsiveness. By integrating chemical reactions, hydrogels acquire dynamic and tunable responsiveness to external stimuli through chemo‐mechanical coupling, expanding their potential in emerging applications. However, capturing their transient behavior remains challenging due to the complex interplay of chemical reactions, solvent transport, and polymer network deformation. Classical theories capture equilibrium swelling but fail to describe time‐dependent phenomena. To address this, a time‐dependent continuum model is developed that explicitly couples these processes. Volume phase transition in hydrogels with homogeneous chemical reactions is investigated, then the effects of reaction kinetics on these transitions are analyzed. The coupling of these mechanisms is further explored through a study of transient mechanical instabilities. To illustrate the impact of distinct reaction and diffusion timescales, a photo‐active gripper is studied for robotic applications. Finally, a photo‐active microswimmer that exhibits non‐reciprocal motion is proposed to highlight the solvent diffusion for locomotion at the micro‐ and nano‐ scales. The work establishes that transient dynamics of chemo‐mechanical hydrogels generate functions not accessible by steady state models and provides a predictive platform for designing adaptive materials in emerging applications.

chemo-mechanical coupling↗
DOE OSTI2024

Functional stimuli-responsive polymers on micro- and nano-patterned interfaces

Micro- and nano-patterned surfaces offer precise control over morphology and chemical composition, enhancing the stability, durability, and functionality of coating materials. When combined with stimuli-responsive polymers, these surfaces gain dynamic adaptability, enabling reversible binding, reusable sensing, and selective molecular capture. Furthermore, while recent review articles have explored various aspects of stimuli-responsive materials, from hydrogel patterns for bioanalytical applications to shape-morphing hydrogels for soft robotics and sensors, a comprehensive review focused on the integration of smart polymers with micro- or nano-patterned interfaces remains absent. This review addresses key surface patterning techniques, including soft lithography, colloidal lithography, and polymer brush photolithography, as well as advances in surface-initiated polymerization methods, such as surface-initiated controlled radical polymerization (SI-CRP). In addition, we discuss recent progress in integrating stimuli-responsive polymers with patterned surfaces to create advanced, functional materials.

Colloidal lithography↗
DOE OSTI2026

Pyrodictium abyssi AbpX reveals a calcium-responsive family of microbial biomatrix proteins that form thermostable hydrogels

Evolutionary pressure on microbial communities propagating under extreme environmental conditions often results in unique structural adaptations to promote cell survival. In this work, we report an investigation of AbpX, a biomatrix protein identified in cultures of the hyperthermophilic archaeon Pyrodictium abyssi. Under ex vivo and in vitro conditions, AbpX assembles into a paracrystalline lattice composed of semiflexible fibrils. CryoEM analysis of recombinant AbpX fibrils reveals that the precursor protein polymerizes through donor strand complementation (DSC), a process previously reported for chaperone-usher fimbriae in Gram-negative bacteria. Unlike the latter DSC protein polymers, AbpX undergoes chaperone-free polymerization in the presence of calcium ions, which are sequestered at the donor strand-acceptor groove interface between protomers in the fibril. Using a combination of cryoEM and crystallographic information, a structural model is proposed for the AbpX lattice that provides insight into its potential role in biofilm formation. These findings suggest that calcium ion coordination may contribute to fibril assembly and preorganize fibrils for incorporation into the protein lattice. Bioinformatic analysis indicates that AbpX exemplifies a distinct and broadly distributed clade of calcium ion responsive biomatrix proteins within the TasA superfamily that can be fabricated into hydrogel biomaterials in vitro under environmentally benign conditions.

59 BASIC BIOLOGICAL SCIENCES↗