Chemo-Mechanically Regulated Oscillation of an Enzymatic Reaction

Chemo-Mechanically Regulated Oscillation of an Enzymatic Reactio

Chemo-Mechanically Regulated Oscillation of an Enzymatic Reaction

Chemo-Mechanically Regulated Oscillation of an Enzymatic Reactio

Harnessing Cooperative Interactions between Thermoresponsive Aptamers and Gels To Trap and Release Nanoparticles

We use computational modeling to design a device that can controllably trap and release particles in solution in response to variations in temperature. The system exploits the thermoresponsive properties of end-grafted fibers and the underlying gel substrate. The fibers mimic the temperature-dependent behavior of biological aptamers, which form a hairpin structure at low temperatures (T) and unfold at higher T, consequently losing their binding affinity. The gel substrate exhibits a lower critical solution temperature and thus, expands at low temperatures and contracts at higher T. By developing a new dissipative particle dynamics simulation, we examine the behavior of this hybrid system in a flowing fluid that contains buoyant nanoparticles. At low T, the expansion of the gel causes the hairpin-shaped fibers to extend into the path of the fluid-driven particle. Exhibiting a high binding affinity for these particles at low temperature, the fibers effectively trap and extract the particles from the surrounding solution. When the temperature is increased, the unfolding of the fiber and collapse of the supporting gel layer cause the particles to be released and transported away from the layer by the applied shear flow. Since the temperature-induced conformational changes of the fiber and polymer gel are reversible, the system can be used repeatedly to “catch and release” particles in solution. Our findings provide guidelines for creating fluidic devices that are effective at purifying contaminated solutions or trapping cells for biological assays

Biomimetic Hydrogel Composites for Soil Stabilization and Contaminant Mitigation

We have developed a novel method to synthesize a hyper-branched biomimetic hydrogel network across a soil matrix to improve the mechanical strength of the loose soil and simultaneously mitigate potential contamination due to excessive ammonium. This method successfully yielded a hierarchical structure that possesses the water retention, ion absorption, and soil aggregation capabilities of plant root systems in a chemically controllable manner. Inspired by the robust organic–inorganic composites found in many living organisms, we have combined this hydrogel network with a calcite biomineralization process to stabilize soil. Our experiments demonstrate that poly­(acrylic acid) (PAA) can work synergistically with enzyme-induced carbonate precipitation (EICP) to render a versatile, high-performance soil stabilization method. PAA-enhanced EICP provides multiple benefits including lengthening of water supply time, localization of cementation reactions, reduction of harmful byproduct ammonium, and achievement of ultrahigh soil strength. Soil crusts we have obtained can sustain up to 4.8 × 10³ kPa pressure, a level comparable to cementitious materials. An ammonium removal rate of 96% has also been achieved. These results demonstrate the potential for hydrogel-assisted EICP to provide effective soil improvement and ammonium mitigation for wind erosion control and other applications

Biomimetic Hydrogel Composites for Soil Stabilization and Contaminant Mitigation

We have developed a novel method to synthesize a hyper-branched biomimetic hydrogel network across a soil matrix to improve the mechanical strength of the loose soil and simultaneously mitigate potential contamination due to excessive ammonium. This method successfully yielded a hierarchical structure that possesses the water retention, ion absorption, and soil aggregation capabilities of plant root systems in a chemically controllable manner. Inspired by the robust organic–inorganic composites found in many living organisms, we have combined this hydrogel network with a calcite biomineralization process to stabilize soil. Our experiments demonstrate that poly­(acrylic acid) (PAA) can work synergistically with enzyme-induced carbonate precipitation (EICP) to render a versatile, high-performance soil stabilization method. PAA-enhanced EICP provides multiple benefits including lengthening of water supply time, localization of cementation reactions, reduction of harmful byproduct ammonium, and achievement of ultrahigh soil strength. Soil crusts we have obtained can sustain up to 4.8 × 10³ kPa pressure, a level comparable to cementitious materials. An ammonium removal rate of 96% has also been achieved. These results demonstrate the potential for hydrogel-assisted EICP to provide effective soil improvement and ammonium mitigation for wind erosion control and other applications

Visualizing Morphogenesis through Instability Formation in 4‑D Printing

Heterogeneous growth in a myriad of biological systems can lead to the formation of distinct morphologies during the maturation processes of different species. We demonstrate that the distinct circumferential buckling observed in pumpkins can be reproduced by a core–shell barrel structure using four-dimensional (4D) printing, taking advantage of digital light processing (DLP)-based three-dimensional (3D) printing and stimulus-responsive hydrogels. The mechanical mismatch between the stiff core and compliant shell results in buckling instability on the surface. The initiation and development of the buckling are governed by the ratio of core/shell radius, the ratio of core/shell swelling ratios, and the mismatch between the core and shell in stiffness. Furthermore, the rigid core not only acts as a source of circumferential confinement but also sets a boundary at the poles of the entire structure. The heterogeneous structures with controllable buckling geometrically and structurally behave much like plants’ fruits. This replicates the biological morphologic change and elucidates the general mechanism and dynamics of the complex instability formation of heterogeneous 3D objects

Toward Rapid Detection of Trace Lead and Cadmium by Anodic Stripping Voltammetry in Complex Wastewater Streams

Heavy metals (HMs), such as lead (Pb) and cadmium (Cd), in municipal wastewater (MWW) limit its use as an alternative water resource. Therefore, monitoring HM concentrations in MWW is critical to evaluating potential reuse applications. However, current metal detection methods rely on grab-sampling and analysis on complicated laboratory-based analytical chemistry instruments, limiting sampling frequency. Anodic stripping voltammetry (ASV) is a promising measurement alternative. However, HMs in MWW are found as complexes and/or sorbed onto particles, and are thus not detectable by ASV. In this study, we develop a processing method that enables the detection of HMs using ASV. In this method, HM-containing MWW is pretreated by either vacuum ultraviolet (VUV)/H2O2(Cd) or a strong acid (Pb), which releases the bound HMs. HMs are then accurately detected and quantified using ASV by utilizing a bismuth subcarbonate/reduced graphene oxide nanocomposite incorporated in a Nafion matrix electrode. The resulting sensing process is able to detect trace concentrations of Cd and Pb in both synthetic and real MWW samples. Detection results were benchmarked against state-of-the-art metal detection methods, and were found to be highly accurate (>88%). This pretreatment and detection method enables utilities and end-users to frequently monitor HM concentrations in complex streams

All-Fabric Capacitive Pressure Sensors with Piezoelectric Nanofibers for Wearable Electronics and Robotic Sensing

Flexible pressure sensors are increasingly sought after for applications ranging from physiological signal monitoring to robotic sensing; however, the challenges associated with fabricating highly sensitive, comfortable, and cost-effective sensors remain formidable. This study presents a high-performance, all-fabric capacitive pressure sensor (AFCPS) that incorporates piezoelectric nanofibers. Through the meticulous optimization of conductive fiber electrodes and P(VDF-TrFE) nanofiber dielectric layers, the AFCPS exhibits exceptional attributes such as high sensitivity (4.05 kPa–1), an ultralow detection limit (0.6 Pa), an extensive detection range (∼100 kPa), rapid response time (14,000 cycles). The sensor’s porous structure enhances its compressibility, while its piezoelectric properties expedite charge separation, thereby increasing the interface capacitance and augmenting overall performance. These features are elucidated further through multiphysical field-coupling simulations and experimental testing. Owing to its comprehensive superior performance, the AFCPS has demonstrated its efficacy in monitoring human activity and physiological signals, as well as in discerning soft robotic grasping movements. Additionally, we have successfully implemented multiple AFCPS units as pressure sensor arrays to ascertain spatial pressure distribution and enable intelligent robotic gripping. Our research underscores the promising potential of the AFCPS device in wearable electronics and robotic sensing, thereby contributing significantly to the advancement of high-performance fabric-based sensors

Photoinduced Dual Shape Programmability of Covalent Adaptable Networks with Remarkable Mechanical Properties

As classic shape memory polymers featuring shape reconfiguration of temporary state, covalent adaptable networks containing reversible bonds can enable permanent-state reconfigurability through topological rearrangement via dynamic bond exchange. Yet, such an attractive dual shape programmability is limited by the actuation mode of direct heat transfer and poor mechanical properties, restricting its control precision and functionality. Herein, we presented a method to create nanocomposites with photomodulated dual shape programmability and remarkable mechanical properties leading the fields of covalent adaptable networks. MXene, whose photothermal efficiency was revealed to be regulated by the etching method and delamination, was introduced into polyurethane networks. Upon adjusting the light intensity, the dual shape programmability of both permanent and temporary states could be accomplished, which exhibited potential in information recognition, photowriting paper, etc. Furthermore, owing to the dynamic transcarbamoylation at elevated temperatures, such a phototriggered dual shape programmability could be maintained after the self-healing and reprocessing

Photoinduced Dual Shape Programmability of Covalent Adaptable Networks with Remarkable Mechanical Properties

As classic shape memory polymers featuring shape reconfiguration of temporary state, covalent adaptable networks containing reversible bonds can enable permanent-state reconfigurability through topological rearrangement via dynamic bond exchange. Yet, such an attractive dual shape programmability is limited by the actuation mode of direct heat transfer and poor mechanical properties, restricting its control precision and functionality. Herein, we presented a method to create nanocomposites with photomodulated dual shape programmability and remarkable mechanical properties leading the fields of covalent adaptable networks. MXene, whose photothermal efficiency was revealed to be regulated by the etching method and delamination, was introduced into polyurethane networks. Upon adjusting the light intensity, the dual shape programmability of both permanent and temporary states could be accomplished, which exhibited potential in information recognition, photowriting paper, etc. Furthermore, owing to the dynamic transcarbamoylation at elevated temperatures, such a phototriggered dual shape programmability could be maintained after the self-healing and reprocessing