Latest ArticlesCO2 capture is considered as one of the most ideal strategies for solving the environmental issues and against global warming. Recently, experimental evidence has suggested that aluminum double bond (dialumene) species can capture CO2 and further convert it into value-added products. However, the catalytic application of these species is still in its infancy. Both the dynamics mechanism of CO2 fixation and the detailed structures of catalytic intermediates are not well understood. In this work, we investigate the structure dependent resonance Raman (RR) signals for different reaction intermediates. Ab-initio simulations of spontaneous resonance Raman (spRR) and time-domain stimulated resonance Raman (stRR) give spectral signatures correlated to the existence of different intermediates during the CO2-dialumene binding process. The unique Raman vibronic features contain rich structural information with high temporal resolution, enabling to monitor the transient catalytic intermediates under reaction conditions. Our work shows that RR can be used to monitor intermediates during the dialumene based CO2 capture reaction. The spectral features not only provide insight into the structural information of intermediate species, but also allow a deeper understanding of the dynamical details of this kind of catalytic process.
Li-O2 batteries (LOBs) have been perceived as the most potential clean energy system for fast-growing electric vehicles by reason of their environmentally friendlier, high energy density and high reversibility. However, there are still some issues limiting the practical application of LOBs, such as the large gap between the actual capacity level and the theoretical capacity, low rate performance as well as short cycle life. Herein, hollow CeO2/Co3O4 polyhedrons have been synthesized by MOF template with a simple method. And it is was further served as a cathode catalyst in Li-O2 batteries. By means of the synergistic effect of two different transition metal oxides, nano-sized hollow porous CeO2/Co3O4 cathode obtained better capacity and cycle performance. As a result, excellent cyclability of exceeding 140 and 90 cycles are achieved at a fixed capacity of 600 and 1000 mAh/g, respectively. The successful application of this catalyst in LOBs offers a novel route in the aspect of the synthesis of other hollow porous composite oxides as catalysts for cathodes in LOBs systems by the MOF template method.
Owing to excellent light absorption and high activity for oxygen evolution, monoclinic bismuth vanadate (BiVO4) is regarded as an ideal candidate for photocatalytic water splitting. However, its application is limited by the large particle size in micrometer scale, as well as the slightly positive conduction band. In this work, we successfully synthesized nano-BiVO4 with particle size ranged from 27 nm to 57 nm by wet chemical method based on electrostatic spinning method. Unlike bulk BiVO4, the nano-sized BiVO4 possesses the ability to generate hydrogen by water splitting, and the activity could reach up to 1.66 μmol h−1g−1 with the assistance of Pt. The enhanced activity is mainly attributed to the improvements resulted from reduced particle size, which includes elevated conduction band, enlarged specific surface area and promoted charge separation. This work provides a simple method for synthesizing photocatalyst with small particle size and high yield.
An efficient and facile method for C–H amination of quinoxalinones with heteroaromatic amines under metal-free conditions has been described. In the presence of hypervalent PIDA reagent, the desired products with various groups were obtained with moderate to high yields.
Developing low toxicity and multifunctional theranostic nanoplatform is the key for precise cancer diagnosis and treatment. Herein, an inorganic-organic hybrid nanocomposite is designed by modifying zirconium dioxide (ZrO2) with polydopamine (PDA) followed by doping Mn2+ ions and functionalizing with Tween 20 (Tween-ZrO2@PDA-Mn2+) for multimodal imaging and chemo-photothermal combination therapy. The as-prepared nanocomposite exhibits good biocompatibility in vitro and in vivo. Specifically, it can be employed as a multifunctional platform not only for computed tomography (CT) imaging and T1-weighted magnetic resonance (MR) imaging, but also for efficient chemotherapeutic drug doxorubicin hydrochloride (DOX) loading. Importantly, because of the pronounced photothermal conversion performance and controllable DOX release ability triggered by the near-infrared (NIR) irradiation and acidic pH, the synergistic effect between photothermal therapy and chemotherapy results in an enhanced cancer treatment efficacy in vivo. Our work provides a high-performance inorganic-organic hybrid nanotheranostic platform for chemo-photothermal cancer therapy guided by CT and MR imaging.
Constructing a heterojunction photocatalyst is a significant method to enhance photocatalytic activity because it can promote the separation of photogenerated carriers. Herein, amorphous/crystalline contact Bi2S3/Bi4O7 heterostructure was successfully synthesized by in-situ sulfidation of Bi4O7. The amorphous Bi2S3 is diffused on the surface of Bi4O7 rod, enhancing the visible light response and improving the transport of photogenerated carriers. Various characterizations confirm that the rapid separation of photogenerated carriers leads to increased photocatalytic performance. The optimized Bi2S3/Bi4O7 heterostructure photocatalyst (BiS-0.15) exhibits the highest Cr(VI) reduction (0.01350 min−1) and RhB oxidation (0.08011 min−1) activity, which is much higher than that of pure Bi4O7 and Bi2S3/Bi4O7 mixture under visible light irradiation. This work provides new insights into the construction of efficient novel photocatalysts.
To enhance the photodegradation ability of CeO2 for organic dyes, an effective strategy is to introduce oxygen vacancies (Vo). In general, the introduced Vo are simultaneously present both on the surface and in the bulk of CeO2. The surface oxygen vacancies (Vo-s) can decrease the band gap, thus enhancing light absorption to produce more photogenerated e− for photodegradation. However, the bulk oxygen vacancies (Vo-b) will inhibit photocatalytic activity by increasing the recombination of photogenerated e− and Vo-b. Therefore, regulating the concentrations of Vo-s to Vo-b is a breakthrough for achieving the best utilization of photogenerated e− during photodegradation. We used an easy hydrothermal method to achieve tunable concentrations of Vo-s to Vo-b in CeO2 nanorods. The optimized CeO2 presents a 70.2% removal of rhodamine B after 120 min of ultraviolet−visible light irradiation, and a superior photodegradation performance of multiple organics. This tuning strategy for Vo also provides guidance for developing other advanced metal-oxide semiconductor photocatalysts for the photodegradation of organic dyes.
Sulfoxonium ylides as carbene precursors couple smoothly with thioureas in the presence of 5 mol% of rhodium(Ⅱ) acetate dimmer via carbenoid insertion to afford the corresponding 2-aminothiazoles with high chemoselectivity, providing a facile and efficient approach to access a variety of 2-aminothiazole derivatives with good functional groups tolerance.
Lipid droplets (LDs) are intracellular lipid-metabolism organelles that involved in many physiological processes, metabolic disorders as well as diseases such as atherosclerosis. However, the specific probes that can visually locate abnormal LDs-rich tissues and track LDs-associated behavior to the naked eye with adequate biosafety still are rare. Herein, we develop a new design strategy of LDs-targeted probe based on the solvatochromism of coumarin derivatives. The results revealed that the emission wavelength of coumarin fluorophores gradually red shift in different solvents with increasing polarity, while absorption wavelength almost unchanged. As a result, the enlarged stokes shift of coumarin was emerged from oil to water. Furthermore, properly reducing water solubility and adding electronic donor at the structure of coumarins can enlarge this type of solvatochromism. This discovery was utilized to develop suitable probe for the image of LDs and LDs-rich tissues with high resolution and biosafety. Therefore, LDs-associated behavior was visible to the naked eye during the process of lipophagy and atherosclerosis. We deem that the developed probe here offers a new possibility to accurately diagnosis and analyse LDs-related diseases in clinic and preclinical study.
Living-cell imaging demands high specificity, sensitivity, and minimal background interference to the targets of interest. However, developing a desirable imaging probe that can possess all the above features is still challenging. The bioorthogonal surface-enhanced Raman scattering (SERS) imaging has been recently emerged through utilizing Raman reporters with characteristic peaks in Raman-silent region of cells (1800-2800 cm-1), which opens a revolutionary avenue for living-cell imaging with multiplexing capability. In this review, we focus on the recent advances in the technology development and the biological and biomedical applications of the living-cell bioorthogonal SERS imaging technique. After introduction of fundamental principles for bioorthogonal tag or label, we present applications for visualization of various intracellular components and environment including proteins, nucleic acids, lipids, pH and hypoxia, even for cancer diagnosis in tissue samples. Then, various bioorthogonal SERS imaging-guided therapy strategies have been discussed such as phototherapy and surgery. In conclusion, this strategy has great potential to be a flexible and robust tool for visualization detection and diseases diagnosis.
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