Programmable locomotion of responsive hydrogels has gained increasing attention for potential applications in soft robotics, microfluidic components, actuators, and artificial muscle. Modulation of ...hydrogel pore structures is essential for tailoring their mechanical strength, response speeds, and motion behaviors. Conventional methods forming hydrogels with homogeneous or stepwise‐distributed pore structures are limited by the required compromise to simultaneously optimize these aspects. Here, a heterobifunctional crosslinker enabled hydrothermal process is introduced to synthesize responsive hydrogels with well‐defined gradient pore construction. According to gradient porosity controls, the hydrogels simultaneously exhibit rapid responses to external stimuli, high elasticity/compressibility, and programmable locomotion capability. By incorporating polypyrrole nanoparticles as photothermal transducers, photo/thermal responsive composite hydrogels are formed to enable programmable control of locomotion such as bending, curving, twisting, and octopus‐like swimming under near‐infrared laser stimulation. The tunable pore structures, mechanical properties, and locomotion of this new class of materials make these gradient porous hydrogels potentially suitable for a variety of applications.
Gradient porous elastic hydrogels with rapid and programmable locomotion to thermal‐/photostimulation are obtained through an effective hydrothermal route. According to the gradient porosity control, the hydrogels simultaneously exhibit rapid responses, high elasticity, and anisotropic locomotion. The hydrothermally induced hydrogelation mechanism is applicable to other thermal‐responsive monomers and crosslinkers, opening new avenues for modulating the pore structures of soft materials.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
The detection of ultratrace analytes is highly desirable for the non‐invasive monitoring of human diseases. However, a major challenge is fast, naked‐eye, high‐resolution ultratrace detection. ...Herein, a rectangular 3D composite photonic crystal (PC)‐based optoelectronic device is first designed that combines the sensitivity‐enhancing effects of PCs and optoelectronic devices with fast and real‐time digital monitoring. A crack‐free, centimeter‐scale, mechanically robust ellipsoidal composite PCs with sufficient hardness and modulus, even exceeding most plastics and aluminum alloys, are developed. The high mechanical strength of ellipsoidal composite PCs allows them to be hand‐machined into rectangular geometries that can be conformally covered with the centimeter‐scale flat light‐detection area without interference from ambient light, easily integrating 3D composite PC‐based optoelectronic devices. The PC‐based device's signal‐to‐noise ratio increases dramatically from original 30–40 to ≈60–70 dB. Droplets of ultratrace analytes on the device are identified by fast digital readout within seconds, with detection limits down to 5 µL, enabling rapid identification of ultratrace glucose in artificial sweat and diabetes risk. The developed 3D PC‐based sensor offers the advantages of small size, low cost, and high reliability, paving the way for wider implementation in other portable optoelectronic devices.
A photonic crystal‐based optoelectronic device is developed for rapid and real‐time digital monitoring of ultratrace analytes with detection limits down to 5 µL, which is highly desirable for the non‐invasive monitoring of human diseases, such as the quick identification of diabetes from ultratrace glucose in sweat.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
In nature, individual cells contain multiple isolated compartments in which cascade enzymatic reactions occur to form essential biological products with high efficiency. Here, we report a ...cell-inspired design of functional hydrogel particles with multiple compartments, in which different enzymes are spatially immobilized in distinct domains that enable engineered, one-pot, tandem reactions. The dense packing of different compartments in the hydrogel particle enables effective transportation of reactants to ensure that the products are generated with high efficiency. To demonstrate the advantages of micro-environmental modifications, we employ the copolymerization of acrylic acid, which leads to the formation of heterogeneous multi-compartmental hydrogel particles with different pH microenvironments. Upon the positional assembly of glucose oxidase and magnetic nanoparticles, these hydrogel particles are able to process a glucose-triggered, incompatible, multistep tandem reaction in one pot. Furthermore, based on the high cytotoxicity of hydroxyl radicals, a glucose-powered therapeutic strategy to kill cancer cells was approached.Cells contain isolated compartments where cascade enzymatic biochemical reactions occur to form essential biological products with high efficiency. Here the authors produce functional hydrogel particles with multiple compartments via microfluidics that contain spatially immobilized natural enzymes in distinct domains for one-pot, tandem reactions.
Detecting and analyzing pathogenic bacteria in an effective and reliable manner is crucial for the diagnosis of acute bacterial infection and initial antibiotic therapy. However, the precise labeling ...and analysis of bacteria at the single‐bacterium level are a technical challenge but very important to reveal important details about the heterogeneity of cells and responds to environment. This study demonstrates an optical strategy for single‐bacterium labeling and analysis by the cotrapping of single upconversion nanoparticles (UCNPs) and bacteria together. A single UCNP with an average size of ≈120 nm is first optically trapped. Both ends of a single bacterium are then trapped and labeled with single UCNPs emitting green light. The labeled bacterium can be flexibly moved to designated locations for further analysis. Signals from bacteria of different sizes are detected in real time for single‐bacterium analysis. This cotrapping method provides a new approach for single‐pathogenic‐bacterium labeling, detection, and real‐time analysis at the single‐particle and single‐bacterium level.
Single‐bacterium labeling and analysis are realized by optical connecting of single upconversion nanoparticles and bacteria using an optical cotrapping method. The labeled single bacterium can be moved to designated locations in 3D for further analysis, and the signal from the labeled single bacterium can be detected in real time for single‐bacteria analysis.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Many living organisms undergo conspicuous or abrupt changes in body structure, which is often accompanied by a behavioral change. Inspired by the natural metamorphosis, robotic systems can be ...designed as reconfigurable to be multifunctional. Here, a tissue‐engineered transformable robot is developed, which can be remotely controlled to assume different mechanical structures for switching locomotive function. The soft robot is actuated by a muscular tail fin that emulates the swimming of whales and works as a cellular engine powered by the synchronized contraction of striated cardiac microtissue constructs. For a transition of locomotive behavior, the robot can be optically triggered to transform from a spread to a retracted form, which effectively changes the bending stiffness of the tail fins, thus minimizing the propulsion output from the “tail fin” and effectively switching off the engine. With the unprecedented controllability and responsiveness, the transformable robot is implemented to work as a cargo carrier for programmed delivery of chemotherapeutic agents to selectively eradicate cancer cells. It is believed that the realization of the transformable concept paves a pathway for potential development of intelligent biohybrid robotic systems.
A tissue‐engineered transformable robot is developed, which can be remotely controlled to assume different mechanical structures for switching locomotive functionality. With the unprecedented controllability and responsiveness, the transformable robot can be implemented for programmed eradication of cancer cells for instance. This design concept paves the way for the potential development of intelligent biohybrid robotic systems.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Reactivation of T cell immunity by PD-1/PD-L1 immune checkpoint blockade has been shown to be a promising cancer therapeutic strategy. However, PD-L1 immunohistochemical readout is inconsistent with ...patient response, which presents a clinical challenge to stratify patients. Because PD-L1 is heavily glycosylated, we developed a method to resolve this by removing the glycan moieties from cell surface antigens via enzymatic digestion, a process termed sample deglycosylation. Notably, deglycosylation significantly improves anti-PD-L1 antibody binding affinity and signal intensity, resulting in more accurate PD-L1 quantification and prediction of clinical outcome. This proposed method of PD-L1 antigen retrieval may provide a practical and timely approach to reduce false-negative patient stratification for guiding anti-PD-1/PD-L1 therapy.
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•N-linked glycosylation of PD-L1 hinders its recognition by PD-L1 antibodies•Removal of glycosylation enhances anti-PD-L1 signal in a variety of bioassays•Patient sample deglycosylation prevents false-negative detection of PD-L1•Deglycosylated PD-L1 is a more reliable biomarker to guide immunotherapy
Histological detection of PD-L1 may guide therapy with anti-PD-1/PD-L1 antibodies but some PD-L1-negative tumors respond to these treatments. Lee et al. show that enzymatic deglycosylation of tissue sections improves PD-L1 detection and its predictive value, and could potentially impact patient stratification.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Secreted proteins determine a range of cellular functionalities correlated with human health and disease progression. Because of cell heterogeneity, it is essential to measure low abundant protein ...secretions from individual cells to determine single‐cell activities. In this study, an integrated platform consisting of smart hydrogel immunosensors for the sensitive detection of single‐cell secretions is developed. A single cell and smart hydrogel microparticles are encapsulated within a droplet. After incubation, target secreted proteins from the cell are captured in the smart hydrogel particle for immunoassay. The temperature‐induced volume phase transition of the hydrogel biosensor allows the concentration of analytes within the gel matrix to increase, enabling high‐sensitivity measurements. Distinct heterogeneity for live cell secretions is determined from 6000 cells within 1 h. This method is tested for low abundant essential secretions, such as interleukin‐6, interleukin‐8, and monocyte chemoattractant protein‐1 secretions of both suspended cells (HL60) and adherent cells (MCF7 and MDA‐MB‐231). This platform is highly flexible and can be used to simultaneously measure a wide range of clinically relevant cellular secretions; it thus represents a novel tool for precise biological assays.
An integrated platform where single cells are encapsulated with smart hydrogel immunosensors within droplets is developed. Temperature‐induced volume phase transition of poly (N‐isopropylacrylamide) hydrogel particles allows analyte concentration within the gel matrix, enabling rapid signal amplification. With this platform, live single‐cell secretions of the multiple cytokines are analyzed, revealing distinct single‐cell secretion heterogeneity.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Achieving efficient photon upconversion under low irradiance is not only a fundamental challenge but also central to numerous advanced applications spanning from photovoltaics to biophotonics. ...However, to date, almost all approaches for upconversion luminescence intensification require stringent controls over numerous factors such as composition and size of nanophosphors. Here, we report the utilization of dielectric microbeads to significantly enhance the photon upconversion processes in lanthanide-doped nanocrystals. By modulating the wavefront of both excitation and emission fields through dielectric superlensing effects, luminescence amplification up to 5 orders of magnitude can be achieved. This design delineates a general strategy to converge a low-power incident light beam into a photonic hotspot of high field intensity, while simultaneously enabling collimation of highly divergent emission for far-field accumulation. The dielectric superlensing-mediated strategy may provide a major step forward in facilitating photon upconversion processes toward practical applications in the fields of photobiology, energy conversion, and optogenetics.
Monodisperse magnetic particles are templated from double emulsions formed using sequential flow‐focus drop formation. The microfluidic drop formation allows the particles to be formed with high ...monodispersity and with consistently anisotropic internal structure. This structural anisotropy gives rise to magnetic anisotropy, allowing the particles to be rotated by a magnetic field.
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