Nanomedicine constructed by therapeutics has unique and irreplaceable advantages in biomedical applications, especially in drug delivery for cancer therapy. The strategy, however, used to construct ...the therapeutics‐based nanomedicines with tumor microenvironmental factor responsiveness is still sophisticated. In this study, an easy‐operating procedure is used to construct a therapeutics‐based nanosystem with active tumor‐targeting, enhanced penetration, and stimuli‐responsive drug release behavior as well as programmed cell death‐1/programmed cell death‐ligand 1 (PD‐1/PD‐L1) blockading mediated immunomodulation to enhance tumor immunotherapy. The matrix metalloproteinase‐2 responsive peptide with the existence of Lyp‐1 sequence contributes to the success of active tumor‐targeting and the enhancement of the penetration of the nanoparticles in tumor tissue. The obtained nanosystem strikingly inhibits the primary tumor growth in the first 24 h (more than 97.5% of tumor cells are inhibited), and total inhibition can be achieved with the combination of photothermal therapy. IR820, which is served as the carrier for the therapeutics, is used as a photosensitizer for photothermal therapy. The progress and aggression of distal tumor has further been alleviated by a d‐peptide which is an antagonist for PD‐1/PD‐L1 blockage. Therefore, a therapeutics‐constructed multifunctional nanosystem is provided to realize a combinational therapeutic strategy to enhance the therapeutic outcome.
An easy‐operating procedure is used to construct a therapeutics‐based nanosystem with active tumor‐targeting, enhanced penetration, and stimuli‐responsive drug release behavior as well as programmed cell death‐1/programmed cell death‐ligand 1 (PD‐1/PD‐L1) blockading‐mediated immunomodulation to enhance tumor immunotherapy. This tumor microenvironment‐responsive peptide is used for targeting ligands as well as blockage for PD‐1/PD‐L1.
High‐energy Li‐rich layered cathode materials (≈900 Wh kg−1) suffer from severe capacity and voltage decay during cycling, which is associated with layered‐to‐spinel phase transition and oxygen redox ...reaction. Current efforts mainly focus on surface modification to suppress this unwanted structural transformation. However, the true challenge probably originates from the continuous oxygen release upon charging. Here, the usage of dielectric polarization in surface coating to suppress the oxygen evolution of Li‐rich material is reported, using Mg2TiO4 as a proof‐of‐concept material. The creation of a reverse electric field in surface layers effectively restrains the outward migration of bulk oxygen anions. Meanwhile, high oxygen‐affinity elements of Mg and Ti well stabilize the surface oxygen of Li‐rich material via enhancing the energy barrier for oxygen release reaction, verified by density functional theory simulation. Benefited from these, the modified Li‐rich electrode exhibits an impressive cyclability with a high capacity retention of ≈81% even after 700 cycles at 2 C (≈0.5 A g−1), far superior to ≈44% of the unmodified counterpart. In addition, Mg2TiO4 coating greatly mitigates the voltage decay of Li‐rich material with the degradation rate reduced by ≈65%. This work proposes new insights into manipulating surface chemistry of electrode materials to control oxygen activity for high‐energy‐density rechargeable batteries.
A dielectric inverse spinel‐structured Mg2TiO4 coating on Li‐rich cathode material significantly suppresses the continuous oxygen release, endowing batteries with remarkable cyclability and well‐inhibited voltage decay, e.g., showing a capacity retention of ≈81% and voltage degradation of only 151 mV after 700 cycles, far superior to 44% and 432 mV of the unmodified counterpart.
Soft actuators based on liquid crystal polymer networks (LCNs) have emerged as an exciting research topic due to many envisioned applications in areas such as soft robotics and self‐regulating ...devices. The infatuation stems from the amazing ability of LCNs to display reversible, large amplitude, and complex shape change as well as locomotion upon a stimuli‐triggered phase transition of mesogens between ordered liquid crystal and disordered isotropic state. Among the various stimuli, light arguably is the most attractive choice. Light can easily be adjusted for its wavelength, intensity, or polarization, structured by means of photomasks or interference patterns, and applied to a target remotely and with high spatiotemporal resolution. Indeed, much research effort is dedicated to LCN actuators that are designed to respond to light in many ways, with light being used not only as an external energy source to drive the shape changes or motion of LCN actuators, but also as a versatile tool in their fabrication and reconfiguration. In this Review, recent achievements are highlighted, a number of important issues are discussed, and critical analysis on the use of light in making, reconfiguring, and driving LCN actuators is provided.
Light plays a key role in the development of soft actuators based on liquid crystal polymer networks (LCNs). In this Review, the use of light for their fabrication, reconfiguration, and motion driving is highlighted and analyzed, a number of challenging issues are discussed, and an outlook on the future development is presented.
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•UiO-66-NH2 with different kinds of defects were synthesized.•UiO-66-NH2-LV with ligand vacancy exhibits the best photocatalytic activity.•DFT calculations reveal UiO-66-NH2-LV has ...the lowest sum of Eabs and ELMCT in the photocatalytic process.
Defects in MOFs can benefit light absorption and charge transfer for photocatalytic application, nevertheless, studies on interplay between structural defects and photocatalytic properties of MOFs are in infancy. Herein, a series of UiO-66-NH2 with different kinds of defects were created for regulating CO2 photocatalytic reduction. Theoretical calculations in combination with experimental data verified that the sample with ligand-vacant (UiO-66-NH2-LV) defect performed better than non-defect, missing-cluster and monocarboxylate compensated ones in the photocatalytic CO2 reduction reactions. UiO-66-NH2-LV shows superior photocatalytic activity with the highest CO yield of 30.5 μmol g−1h−1, which is 9.2 times higher than that of the sample with missing-cluster (UiO-66-NH2-MC), as well as the highest quantum yield (QY) of 0.90%. DFT calculations further demonstrate the correlation between discriminative photocatalytic activities in defect structures and tunable electronic properties characterized by absorption energy, Eabs, and charge transfer energy, ELMCT, in the photocatalytic process. The ligand-vacant defect with the lowest sum of Eabs and ELMCT will lower photocatalytic reaction energy barrier in the rate-limiting step among the elementary reaction step during CO2 photoreduction. The insights gained from this study will guide the MOFs defect-engineering for enhancing CO2 photocatalytic capacity.
The engineering of a series of multienzyme‐mimicking covalent organic frameworks (COFs), COF‐909‐Cu, COF‐909‐Fe, and COF‐909‐Ni, as pyroptosis inducers, remodeling the tumor microenvironment to boost ...cancer immunotherapy, is reported. Mechanistic studies reveal that these COFs can serve as hydrogen peroxide (H2O2) homeostasis disruptors to elevate intracellular H2O2 levels, and they not only exhibit excellent superoxide dismutase (SOD)‐mimicking activity and convert superoxide radicals (O2•−) to H2O2 to facilitate H2O2 generation, but also possess outstanding glutathione peroxidase (GPx)‐mimicking activity and deplete glutathione (GSH) to alleviate the scavenging of H2O2. Meanwhile, the outstanding photothermal therapy properties of these COFs can accelerate the Fenton‐like ionization process to facilitate their chemodynamic therapy efficiency. One member, COF‐909‐Cu, can robustly induce gasdermin E (GSDME)‐dependent pyroptosis and remodel the tumor microenvironment to trigger durable antitumor immunity, thus promoting the response rate of αPD‐1 checkpoint blockade and successfully restraining tumor metastasis and recurrence.
A series of multienzyme‐mimicking covalent organic frameworks (COFs) is constructed by dispersing active sites into the COF backbone. In contrast to their corresponding bulk species, these enzyme‐mimicking COFs can serve as H2O2 homeostasis disruptors to elevate intracellular H2O2 levels, thus exhibiting excellent chemodynamic therapy and pyroptosis efficacy, favorable for boosting cancer immunotherapy.
Realizing efficient red/near‐infrared (NIR) electroluminescence (EL) by precisely modulating molecular aggregations of thermally activated delayed fluorescence (TADF) emitters is an attractive ...pathway, yet the molecular designs are elusive. Here, a new approach is proposed to manage molecular aggregation via a mild‐twist acceptor‐donor‐acceptor (A‐D‐A)‐type molecular design. A proof‐of‐concept TADF molecule, QCN‐PhSAC‐QCN, is developed that furnishes a fast radiative rate and obvious aggregation‐induced emission feature. Its emission bands can be facilely shifted from intrinsic yellow to the red/NIR region via fine‐tuning doping levels and molecular aggregates while maintaining elegant photoluminescence quantum yields benefiting from suppressed exciton annihilation processes. As a result, a QCN‐PhSAC‐QCN‐based organic light‐emitting diode (OLED) exhibits a record‐setting external quantum efficiency (EQE) of 39.1% at a doping ratio of 10 wt.%, peaking at 620 nm. Moreover, its nondoped NIR OLED affords a champion EQE of 14.3% at 711 nm and retains outstanding EQEs of 5.40% and 2.35% at current densities of 10 and 100 mA cm−2, respectively, which are the highest values among all NIR‐TADF OLEDs at similar density levels. This work validates the feasibility of such mild‐twist A‐D‐A‐type molecular design for precisely controlling molecular aggregation while maintaining high efficiency, thus providing a promising pathway for high‐performance red/NIR TADF OLEDs.
State‐of‐the‐art red/near‐infrared organic light‐emitting diodes are realized by modulating molecular aggregation based on an intrinsic yellow acceptor‐donor‐acceptor‐type molecule with mild twists. Its doped red device delivers a record‐setting external quantum efficiency (EQE) of 39.1% at 620 nm. Furthermore, its nondoped near‐infrared device also offers a topmost EQE of 14.3% at 711 nm and retains decent EQEs at high current densities.
Electrochemical water splitting in alkaline solution plays a growing role in alternative energy devices due to the need for clean and sustainable energy. However, catalysts that are active for both ...hydrogen evolution and oxygen evolution reactions are rare. Herein, we demonstrate that cobalt phosphide (CoP), which was synthesized via the hydrothermal route and has been shown to have hydrogen evolution activity, is highly active for oxygen evolution. A current density of 10 mA cm–2 was generated at an overpotential of only 320 mV in 1 M KOH for a CoP nanorod-based electrode (CoP NR/C), which was competitive with commercial IrO2. The Tafel slope for CoP NR/C was only 71 mV dec–1, and the catalyst maintained high stability during a 12 h test. This high activity was attributed to the formation of a thin layer of ultrafine crystalline cobalt oxide on the CoP surface.
With the development of manufacturing, machining data applications are becoming a key technological component of enhancing the intelligence of manufacturing. The new generation of machine tools ...should be digitalized, highly efficient, network-accessible and intelligent. An intelligent machine tool (IMT) driven by the digital twin provides a superior solution for the development of intelligent manufacturing. In this paper, a real-time machining data application and service based on IMT digital twin is presented. Multisensor fusion technology is adopted for real-time data acquisition and processing. Data transmission and storage are completed using the MTConnect protocol and components. Multiple forms of HMIs and applications are developed for data visualization and analysis in digital twin, including the machining trajectory, machining status and energy consumption. An IMT digital twin model is established with the aim of further data analysis and optimization, such as the machine tool dynamics, contour error estimation and compensation. Examples of the IMT digital twin application are presented to prove that the development method of the IMT digital twin is effective and feasible. The perspective development of machining data analysis and service is also discussed.
Liquid crystalline network (LCN) actuator normally deforms upon thermally or optically induced order-disorder phase transition, switching once between two shapes (shape 1 in LC phase and shape 2 in ...isotropic state) for each stimulation on/off cycle. Herein, we report an LCN actuator that deforms from shape 1 to shape 2 and then reverses the deformation direction to form shape 3 on heating or under light only, thus completing the shape switch twice for one stimulation on/off cycle. The deformation reversal capability is obtained with a monolithic LCN actuator whose two sides are made to start deforming at different temperatures and exerting different reversible strains, by means of asymmetrical crosslinking and/or asymmetrical stretching. This desynchronized actuation strategy offers possibilities in developing light-fueled LCN soft robots. In particular, the multi-stage bidirectional shape change enables multimodal, light-driven locomotion from the same LCN actuator by simply varying the light on/off times.
Parkinson's disease (PD) is a neurodegenerative disorder and 70-80% of PD patients suffer from gastrointestinal dysfunction such as constipation. We aimed to assess the efficacy and safety of fecal ...microbiota transplantation (FMT) for treating PD related to gastrointestinal dysfunction. We conducted a prospective, single- study. Eleven patients with PD received FMT. Fecal samples were collected before and after FMT and subjected to 16S ribosomal DNA (rDNA) gene sequencing. Hoehn-Yahr (H-Y) grade, Unified Parkinson's Disease Rating Scale (UPDRS) score, and the Non-Motion Symptom Questionnaire (NMSS) were used to assess improvements in motor and non-motor symptoms. PAC-QOL score and Wexner constipation score were used to assess the patient's constipation symptoms. All patients were tested by the small intestine breath hydrogen test, performed before and after FMT. Community richness (chao) and microbial structure in before-FMT PD patients were significantly different from the after-FMT. We observed an increased abundance of Blautia and Prevotella in PD patients after FMT, while the abundance of Bacteroidetes decreased dramatically. After FMT, the H-Y grade, UPDRS, and NMSS of PD patients decreased significantly. Through the lactulose H2 breath test, the intestinal bacterial overgrowth (SIBO) in PD patients returned to normal. The PAC-QOL score and Wexner constipation score in after-FMT patients decreased significantly. Our study profiles specific characteristics and microbial dysbiosis in the gut of PD patients. FMT might be a therapeutic potential for reconstructing the gut microbiota of PD patients and improving their motor and non-motor symptoms.
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