Latest ArticlesIncorporating metal nanoparticles (MNPs) inside metal-organic frameworks (MOFs) demonstrates superior catalytic properties in numerous reactions; however, the size and distribution of MNPs could not be well controlled, resulting in low product selectivity in catalysis by undergoing different catalytic reaction pathways. We report herein a facile strategy for integrating lattice-mismatched MOFs together to fabricate homogeneously distributed “dual-MOFs,” which are the ideal precursors for the preparation of MNPs@MOFs with unique catalytic properties. As a proof of concept, we successfully synthesize a dual-MOF HKUST-1/ZIF-8 for in situ creation of redox-active Cu NPs inside hierarchical porous ZIF-8 under controlled pyrolytic conditions. Combining the advantages of size-tunable Cu NPs in the molecular sieving matrix of ZIF-8, Cu@ZIF-8 demonstrates high activity and selectivity for transformation of alkynes into alkenes without overhydrogenation, which surpasses most of the catalysts in the literature. Therefore, this work paves a new pathway for developing highly efficient and selective heterogeneous catalysts to produce highly value-added chemicals.
This work reports on a compositionally graded heterojunction for photovoltaic application by cooperating fluorine-doped carbon quantum dots (FCQDs in short) into the CsPbI2.5Br0.5 inorganic perovskite layer. Using this CsPbI2.5Br0.5/FCQDs graded heterojunction in conjunction with low-temperature-processed carbon electrode, a power conversion efficiency of 13.53% for 1 cm2 all-inorganic perovskite solar cell can be achieved at AM 1.5G solar irradiation. To the best of our knowledge, this is one of the highest efficiency reported for carbon electrode based all-inorganic perovskite solar cells so far, and the first report of 1 cm2 carbon counter electrode based inorganic perovskite solar cell with PCE exceeding 13%. Moreover, the inorganic perovskite/carbon quantum dot graded heterojunction photovoltaics maintained over 90% of their initial efficiency after thermal aging at 85° for 1056 hours. This conception of constructing inorganic perovskite/FCQDs graded heterojunction offers a feasible pathway to develop efficient and stable photovoltaics for scale-up and practical applications.
Cutting-edge technologies of stretchable, skin-mountable, and wearable electronics have attracted tremendous attention recently due to their very wide applications and promising performances. One direction of particular interest is to investigate novel properties in stretchable electronics by exploring multifunctional materials. Here, we report an integrated strain sensing system that is highly stretchable, rehealable, fully recyclable, and reconfigurable. This system consists of dynamic covalent thermoset polyimine as the moldable substrate and encapsulation, eutectic liquid metal alloy as the strain sensing unit and interconnects, and off-the-shelf chip components for measuring and magnifying functions. The device can be attached on different parts of the human body for accurately monitoring joint motion and respiration. Such a strain sensing system provides a reliable, economical, and ecofriendly solution to wearable technologies, with wide applications in health care, prosthetics, robotics, and biomedical devices.
Since designing efficient tactile sensors for autonomous robots is still a challenge, this paper proposes a perceptual system based on a bioinspired triboelectric whisker sensor (TWS) that is aimed at reactive obstacle avoidance and local mapping in unknown environments. The proposed TWS is based on a triboelectric nanogenerator (TENG) and mimics the structure of rat whisker follicles. It operates to generate an output voltage via triboelectrification and electrostatic induction between the PTFE pellet and copper films (0.3 mm thickness), where a forced whisker shaft displaces a PTFE pellet (10 mm diameter). With the help of a biologically inspired structural design, the artificial whisker sensor can sense the contact position and approximate the external stimulation area, particularly in a dark environment. To highlight this sensor’s applicability and scalability, we demonstrate different functions, such as controlling LED lights, reactive obstacle avoidance, and local mapping of autonomous surface vehicles. The results show that the proposed TWS can be used as a tactile sensor for reactive obstacle avoidance and local mapping in robotics.
Central nervous system diseases commonly occur with the destruction of the blood-brain barrier. As a primary cause of morbidity and mortality, stroke remains unpredictable and lacks cellular biomarkers that accurately quantify its occurrence and development. Here, we identify NeuN+/CD45−/DAPI+ phenotype nonblood cells in the peripheral blood of mice subjected to middle cerebral artery occlusion (MCAO) and stroke patients. Since NeuN is a specific marker of neural cells, we term these newly identified cells as circulating neural cells (CNCs). We find that the enumeration of CNCs in the blood is significantly associated with the severity of brain damage in MCAO mice (). Meanwhile, the number of CNCs is significantly higher in stroke patients than in negative subjects (). These findings suggest that the amount of CNCs in circulation may serve as a clinical indicator for the real-time prognosis and progression monitor of the occurrence and development of ischemic stroke and other nervous system disease.
Benefiting from treating diseases at the genetic level, gene therapy has been considered a new revolution in the biomedical field. However, the extracellular and intracellular barriers during gene transport such as enzymatic degradation and endo-/lysosomal sequestration significantly compromise the therapeutic efficacy. Though photochemical internalization (PCI) has emerged as a promising approach for causing endo-/lysosomal leakage with translocation of the internalized molecules into the cytosol, its effect is still unsatisfactory due to the insufficient light penetration depth. Here, we develop tumor microenvironment-specific enhanced gene delivery by means of ROS generated from the in situ cascaded catalytic reactions in tumors involving GOx-mediated redox reaction and Mn2+-mediated Fenton-like reaction. The efficient enzymatic protection and successful endo-/lysosomal escape of cargo gene complexes have been demonstrated. Moreover, anti-Twist siRNA-loaded G@MMSNs-P exhibit tumor-specific biodegradation, excellent T1-weighted MR imaging, and significant inhibitory effects against breast cancer growth and pulmonary metastasis.
The therapeutic outcomes of noninvasive sonodynamic therapy (SDT) are always compromised by tumor hypoxia, as well as inherent protective mechanisms of tumor. Herein, we report a simple cascade enzymatic approach of the concurrent glucose depletion and intratumoral oxygenation for starvation-sensitized and oxygenation-amplified sonodynamic therapy using a dual enzyme and sonosensitizer-loaded nanomedicine designated as GOD/CAT@ZPF-Lips. In particular, glucose oxidase- (GOD-) catalyzed glycolysis would cut off glucose supply within the tumor, resulting in the production of tumor hydrogen peroxide (H2O2) while causing tumor cells starvation. The generated H2O2 could subsequently be decomposed by catalase (CAT) to generate oxygen, which acts as reactants for the abundant singlet oxygen (1O2) production by loaded sonosensitizer hematoporphyrin monomethyl ether (HMME) upon the US irradiation, performing largely elevated therapeutic outcomes of SDT. In the meantime, the severe energy deprivation enabled by GOD-catalyzed glucose depletion would prevent tumor cells from executing protective mechanisms to defend themselves and make the tumor cells sensitized and succumbed to the cytotoxicity of 1O2. Eventually, GOD/CAT@ZPF-Lips demonstrate the excellent tumoral therapeutic effect of SDT in vivo without significant side effect through the cascade enzymatic starvation and oxygenation, and encouragingly, the tumor xenografts have been found completely eradicated in around 4 days by the intravenous injection of the nanomedicine without reoccurrence for as long as 20 days.
Sensors capable of monitoring dynamic mechanics of tendons throughout a body in real time could bring systematic information about a human body’s physical condition, which is beneficial for avoiding muscle injury, checking hereditary muscle atrophy, and so on. However, the development of such sensors has been hindered by the requirement of superior portability, high resolution, and superb conformability. Here, we present a wearable and stretchable bioelectronic patch for detecting tendon activities. It is made up of a piezoelectric material, systematically optimized from architectures and mechanics, and exhibits a high resolution of with a linearity parameter of . Additionally, a tendon real-time monitoring and healthcare system is established by integrating the patch with a micro controller unit (MCU), which is able to process collected data and deliver feedback for exercise evaluation. Specifically, through the patch on the ankle, we measured the maximum force on the Achilles tendon during jumping which is about 16312 N, which is much higher than that during normal walking (3208 N) and running (5909 N). This work not only provides a strategy for facile monitoring of the variation of the tendon throughout the body but also throws light on the profound comprehension of human activities.
Aggregation-induced emission nanoparticles (AIE NPs) are widely used in the biomedical field. However, understanding the biological process of AIE NPs via fluorescence imaging is challenging because of the strong background and poor penetration depth. Herein, we present a novel dual-modality imaging strategy that combines fluorescence imaging and label-free laser desorption/ionization mass spectrometry imaging (LDI MSI) to map and quantify the biodistribution of AIE NPs (TPAFN-F127 NPs) by monitoring the intrinsic photoluminescence and mass spectrometry signal of the AIE molecule. We discovered that TPAFN-F127 NPs were predominantly distributed in the liver and spleen, and most gradually excreted from the body after 5 days. The accumulation and retention of TPAFN-F127 NPs in tumor sites were also confirmed in a tumor-bearing mouse model. As a proof of concept, the suborgan distribution of TPAFN-F127 NPs in the spleen was visualized by LDI MSI, and the results revealed that TPAFN-F127 NPs were mainly distributed in the red pulp of the spleen with extremely high concentrations within the marginal zone. The in vivo toxicity test demonstrated that TPAFN-F127 NPs are nontoxic for a long-term exposure. This dual-modality imaging strategy provides some insights into the fine distribution of AIE NPs and might also be extended to other polymeric NPs to evaluate their distribution and drug release behaviors in vivo.
Shape-morphing hydrogels can be widely used to develop artificial muscles, reconfigurable biodevices, and soft robotics. However, conventional approaches for developing shape-morphing hydrogels highly rely on composite materials or complex manufacturing techniques, which limit their practical applications. Herein, we develop an unprecedented strategy to edit the shape morphing of monocomponent natural polysaccharide hydrogel films via integrating gradient cross-linking density and geometry effect. Owing to the synergistic effect, the shape morphing of chitosan (CS) hydrogel films with gradient cross-linking density can be facilely edited by changing their geometries (length-to-width ratios or thicknesses). Therefore, helix, short-side rolling, and long-side rolling can be easily customized. Furthermore, various complex artificial 3D deformations such as artificial claw, horn, and flower can also be obtained by combining various flat CS hydrogel films with different geometries into one system, which can further demonstrate various shape transformations as triggered by pH. This work offers a simple strategy to construct a monocomponent hydrogel with geometry-directing programmable deformations, which provides universal insights into the design of shape-morphing polymers and will promote their applications in biodevices and soft robotics.