Load-bearing soft tissues normally show J-shaped stress–strain behaviors with high compliance at low strains yet high strength at high strains. They have high water content but are still tough and durable. By contrast, naturally derived hydrogels are weak and brittle. Although hydrogels prepared from synthetic polymers can be strong and tough, they do not have the desired bioactivity for emerging biomedical applications. Here, we present a thermomechanical approach to replicate the combinational properties of soft tissues in protein-based photocrosslinkable hydrogels. As a demonstration, we create a gelatin methacryloyl fiber hydrogel with soft tissue-like mechanical properties, such as low Young’s modulus (0.1 to 0.3 MPa), high strength (1.1 ± 0.2 MPa), high toughness (9,100 ± 2,200 J/m 3 ), and high fatigue resistance (2,300 ± 500 J/m 2 ). This hydrogel also resembles the biochemical and architectural properties of native extracellular matrix, which enables a fast formation of 3D interconnected cell meshwork inside hydrogels. The fiber architecture also regulates cellular mechanoresponse and supports cell remodeling inside hydrogels. The integration of tissue-like mechanical properties and bioactivity is highly desirable for the next-generation biomaterials and could advance emerging fields such as tissue engineering and regenerative medicine.
more »
« less
This content will become publicly available on March 28, 2026
Carbonization of Butadiene Enables Recyclable Carbon Fiber Polymer Composites
The catalytic conversion of carbon dioxide into polymers via high-energy comonomers offers a sustainable, low-cost, and low-emission approach for developing conveniently manufactured high-performance materials without competing for land-use or food resources. We present the synthesis of poly(amidoamine) polymers stoichiometrically derived from carbon dioxide, butadiene, and amines displaying useful mechanical properties (tensile strength 43 MPa, Young’s modulus 840 MPa, and flexural modulus 2.8 GPa). The low viscosity precursors are applicable to producing carbon fiber reinforced polymers with fiber wetting and rapid network formation (16 minutes at 150°C). This work reveals that internal hydrogen-bonding catalyzes the ring-opening polymerization, and the intramolecular alcohol moiety promotes chemical recyclability in acidic conditions, allowing fiber recovery with <1.0 wt % difference from virgin fiber and monomer in 72% yield.
more »
« less
- Award ID(s):
- 2215940
- PAR ID:
- 10652205
- Publisher / Repository:
- Engage
- Date Published:
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Soft bioelectronic devices exhibit motion-adaptive properties for neural interfaces to investigate complex neural circuits. Here, we develop a fabrication approach through the control of metamorphic polymers’ amorphous-crystalline transition to miniaturize and integrate multiple components into hydrogel bioelectronics. We attain an about 80% diameter reduction in chemically cross-linked polyvinyl alcohol hydrogel fibers in a fully hydrated state. This strategy allows regulation of hydrogel properties, including refractive index (1.37-1.40 at 480 nm), light transmission (>96%), stretchability (139-169%), bending stiffness (4.6 ± 1.4 N/m), and elastic modulus (2.8-9.3 MPa). To exploit the applications, we apply step-index hydrogel optical probes in the mouse ventral tegmental area, coupled with fiber photometry recordings and social behavioral assays. Additionally, we fabricate carbon nanotubes-PVA hydrogel microelectrodes by incorporating conductive nanomaterials in hydrogel for spontaneous neural activities recording. We enable simultaneous optogenetic stimulation and electrophysiological recordings of light-triggered neural activities in Channelrhodopsin-2 transgenic mice.more » « less
-
Characterization of the interphase region in carbon fiber reinforced polymer (CFRP) is challenging because of the length scale involved. The interpretation of measured load-displacement curves using indentation is affected by the lack of analytical solutions that account for the fiber constraint effect. A combination of AFM (Atomic Force Microscopy) based indentation and FE (Finite Element) simulations showed a gradient in the elastic modulus of the interphase evaluated along a radial line from the fiber. 3D FEA (Finite Element Analysis) indicated that fiber constraint effect is significant in the region less than 40 nm away from the fiber. Nonetheless, the apparent rise in elastic modulus due to fiber constraint is limited when compared to the gradient in the elastic modulus of the interphase. Additionally, this technique is used to demonstrate that UV irradiation causes a rapid decrease in the modulus of the region near the fiber due to photocatalytic degradation of carbon fiber but subsequently increases due to high cross-linking. Whereas, the modulus of the matrix at 8 mm away from the fiber decreased by 32% after 24 h of UV irradiation. This indicates that the response of epoxy to UV irradiation is influenced by the proximity to the reinforcement.more » « less
-
Abstract The current electric vehicles (EVs) face many challenges like limited charge capacity, low miles/charge, and long charging times. Herein, these issues are addressed by developing a dual‐function supercapacitor‐based energy‐storing carbon fiber reinforced polymer (e‐CFRP) that can store electrical energy and function as the structural component for the EV's body shell. This is achieved by developing a unique design, vertically aligned graphene sheets attached to carbon fiber electrodes on which different metal oxides are deposited to obtain high‐energy density electrodes. A high‐strength multilayer e‐CFRP assembly is fabricated using an alternate layer patterning configuration of epoxy and polyacrylamide gel electrolyte. The e‐CFRP so developed delivers a high areal energy density of 0.31 mWh cm–2at 0.3 mm thickness and a high tensile strength of 518 MPa, bending strength of 477 MPa, and impact strength of 2666 J m–1. To show its application in EVs, a toy car's body panel is fabricated with e‐CFRP and the toy car is able to operate using the energy stored in its frame. Moreover, when integrated with a solar cell, this composite powers an Internet of Things device, showing its feasibility in communication satellites.more » « less
-
Abstract Semiconducting donor–acceptor (D–A) polymers have attracted considerable attention toward the application of organic electronic and optoelectronic devices. However, a rational design rule for making semiconducting polymers with desired thermal and mechanical properties is currently lacking, which greatly limits the development of new polymers for advanced applications. Here, polydiketopyrrolopyrrole (PDPP)‐based D–A polymers with varied alkyl side‐chain lengths and backbone moieties are systematically designed, followed by investigating their thermal and thin film mechanical responses. The experimental results show a reduction in both elastic modulus and glass transition temperature (Tg) with increasing side‐chain length, which is further verified through coarse‐grained molecular dynamics simulations. Informed from experimental results, a mass‐per‐flexible bond model is developed to capture such observation through a linear correlation betweenTgand polymer chain flexibility. Using this model, a wide range of backboneTgover 80 °C and elastic modulus over 400 MPa can be predicted for PDPP‐based polymers. This study highlights the important role of side‐chain structure in influencing the thermomechanical performance of conjugated polymers, and provides an effective strategy to design and predictTgand elastic modulus of future new D–A polymers.more » « less
An official website of the United States government
