Latest ArticlesEnaminones, which possesses both the nucleophilic enamine as well as electrophilic enone structures, are well known versatile building blocks in organic synthesis. Meanwhile, visible light-mediated reactions have emerged as useful synthetic strategy with enhanced sustainability. Around the last decade, various photochemical transformations of enaminones have been developed to construct cyclic or acyclic compounds. In this review, we describe the recent advances in visible light-mediated chemical transformations of enaminones. Detailed discussion on the reaction mechanism of the related reactions is given to provide guide to the reader. Finally, a summary on the existing challenges and the future outlook towards the development of practical photocatalytic reactions of enaminones is also presented.
In recent years, with the emergence of non-fullerene fused-ring acceptors, power conversion efficiencies (PCEs) of organic solar cells (OSCs) have exceeded 19%. However, compared to inorganic or perovskite photovoltaic cells, a higher voltage loss has become one of the key factors limiting further improvement in the PCEs of OSCs. The ternary/quaternary strategy has been identified as a feasible and effective way to obtain high-efficiency OSCs. In this review, a brief outline is given of the key roles that guest materials played in reducing voltage losses in solar cell devices and a brief look at the future material design and the design of ternary/quaternary systems.
Although it has been developed for many years, nucleic acid aptamer screening technology still fails to be widely used, a considerable part of it is due to the variability of tumor cell morphology, which leads to the use of immortalized cell lines in the laboratory to screen nucleic acid aptamers for recognition ability of tumor cells in the diseased body. To address this, primary cells that can be stably passaged were isolated and extracted from spontaneous tumors of genetically engineered pancreatic ductal adenocarcinoma model mice in this study. Next, an automated screening instrument for nucleic acid aptamers developed autonomously by our group was used to perform efficient aptamer screening using a limited number of cells, and the obtained nucleic acid aptamers were affinity verified at the cellular level. Finally, to answer the question of the cell growth environment difference on the recognition ability of nucleic acid aptamers, we verified its targeting ability to tumors in vivo on a nude mice xenograft tumor model, and further used a common antitumor drug doxorubicin combined with nucleic acid aptamers to verify the drug loading ability of this aptamer combined with the targeting therapeutic ability.
Interface engineering is of great importance to improve the photocatalytic performance. Herein, in-situ formation plasmon Bi/BiOCl nanosheets assembled heterojunction microspheres are fabricated via facile reductive solvothermal approach. The aldehyde group in the DMF structure is used to exert the weak reducing property of the solvent and thus strip out the metal Bi in BiOCl. The metal Bi is anchored on surface of BiOCl firmly due to in-situ formation engineered interface, which could realize efficient charge transfer channel. The resultant Bi/BiOCl heterojunctions assemblies with narrow bandgap of 3.05 eV and mesoporous structure extend the photoresponse to visible light region and could provide sufficient surface active sites. The visible-light-driven photocatalytic degradation of high-toxic norfloxacin for Bi/BiOCl heterojunctions is up to 95.5% within 20 min, representing several times that of pristine BiOCl nanosheets and the physical mixture. It is attributed to the in-situ formation of Bi/BiOCl heterojunctions and surface plasmon resonance (SPR) effect of plasmon Bi promoting charge transfer, and the obvious photothermal effect promoting the photocatalytic reaction, which are verified by experimental and density functional theory (DFT) calculations. This strategy provides ideal perspectives for fabricating metal/semiconductor heterojunctions photocatalysts with high-performance.
Aqueous zinc metal batteries are considered as promising candidates for next-generation electrochemical energy storage devices, especially for large-scale energy storage, due to the advantages of high-safety, high energy density and low cost. As the bridge connecting cathode and anode, electrolyte provides a realistic operating environment. In alkaline and neutral aqueous zinc metal batteries, issues associated with electrolyte and anode are still intractable. In this review, we reveal the development and evolution of electrolytes for aqueous zinc metal batteries from alkaline to neutral via the description of fundamentals and challenges in terms of comparison and connection. We also elaborate the strategies in electrolytes regulation and highlight the basic roles and progresses in additives engineering.
The design and development of energy storage device with high energy/power density has become a research hotspot. Zinc-ion hybrid capacitors (ZHCs) are considered as one of the most promising candidates. However, the application of ZHCs is hindered by their low energy density at high power density due to the unsatisfactory cathode material. In this study, a novel 3D phosphorus-doped carbon nanotube/reduced graphene oxide (P-CNT/rGO) aerogel cathode is synthesized through a synergistic modification strategy of CNT insertion and P doping modification combined with 3D porous design. The as-obtained P-CNT/rGO aerogel cathode manifests significantly increased surface aera, expanded interlayer spacing, and enhanced pseudocapacitance behavior, thus leading to significantly enhanced specific capacitance and superb ions transport performance. The as-assembled ZHC based on P-CNT/rGO cathode delivers a superior energy density of 42.2 Wh/kg at an extreme-high power density of 80 kW/kg and excellent cycle life. In-depth kinetic analyses are undertaken to prove the enhanced pseudocapacitance behavior and exceptional power output capability of ZHCs. Furthermore, the reaction mechanism of physical and chemical adsorption/desorption of electrolyte ions on the P-CNT/rGO cathode is revealed by systematic ex-situ characterizations. This work can provide a valuable reference for developing advanced graphene-based cathode for high energy/power density ZHCs.
Owing to the large exciton binding energy (>100 meV) of most organic materials, the process of exciton dissociation into free electrons and holes is seriously hindered, which plays a key role in the photocatalytic system. In this study, a series of chalcogen (S, Se)-substituted mesoporous covalent organic frameworks (COFs) have been synthesized for enhanced photocatalytic organic transformations. Photoelectrochemical measurements indicate that the introduction of semi-metallic Se atom and the enlargement of conjugation degree can not only reduce the exciton binding energy accelerating the charge separation, but also reduce the band gap of COFs. As a result, the COF-NUST-36 with the lowest exciton binding energy (39.5 meV) shows the highest photocatalytic performance for selective oxidation of amines (up to 98% Conv. and 97.5% Sel.). This work provides a feasible method for designing COFs with high photocatalytic activity by adjusting exciton binding energy.
One of the urgent and challenging topics in diversified sustainable energy conversion is the development of high-performance, low-cost, and well durable catalysts. Cu single-atom catalysts (SACs) have become promising catalysts for diversified sustainable energy conversion due to their capability to maximize the utilization efficiency, acquire modulated electronic structure and optimized binding strength with intermediates. In this review, we have provided an interview of the recent progress achieved in the field of electrocatalysis, photocatalysis, and heterogeneous reaction based on Cu SACs. Started by this review, we have summarized some advanced synthetic strategies for the construction of Cu SACs. Subsequently, the performance-improving strategies are discussed in terms of the coordination environments of the reaction center, reaction mechanism and selectivity, based on free energy diagram and electron structure analysis. Finally, the remaining issues, challenges, and opportunities of Cu SACs are also provided, affording a perspective for future studies. This review not only offers us a deep understanding on the catalytic mechanism of Cu SACs for energy conversion, but also encourages more endeavors in prompting their practical application.
Establishing an effective charge transfer mechanism in carbon nitride (g-C3N4) to enhance its photocatalytic activity remains a limiting nuisance. Herein, the combination design of a single Cu atom with hollow g-C3N4 nanospheres (Cu-N3 structure) has been proven to offer significant opportunities for this crucial challenge. Moreover, this structure endows two pathways for charge transfer in the reaction, namely, the N atoms in the three-dimensional planar structure are only bonded with a single Cu atom, and charge transfer occurs between the plane and the layered structure due to the bending of the interlayered g-C3N4 hollow nanospheres. Notably, Cu-N3 and hollow nanosphere structures have been certified to greatly enhance the efficiency of photogenerated carrier separation and transfer between the layers and planes by ultrafast spectral analysis. As a result, this catalyst possesses unparalleled photocatalytic efficiency. Specifically, the hydrogen production rate up to 2040 µmol h−1 g−1, which is 51 times that of pure C3N4 under visible light conditions. The photocatalytic degradation performance of tetracycline and oxidation performance of benzene is also expressed, with a degradation rate of 100%, a conversion of 97.3% and a selectivity of 99.9%. This work focuses on the structure-activity relationship to provide the possibilities for the development of potential photocatalytic materials.
Bone metastasis, a life-threatening complication of advanced breast cancer, is often accompanied by debilitating pain (cancer-induced bone pain, CIBP) that severely impairs life quality and survival. The concurrent treatment of bone metastases and CIBP remains a clinical challenge because the therapeutic options are limited. In this study, we construct a near-infrared light-activated nano-therapeutic system to meet this conundrum. In detail, sorafenib (SRF) and photosensitizer (chlorin e6, Ce6) are encapsulated into mesoporous hydroxyapatite nanoparticles (HANPs), which are further functionalized with hyaluronic acid (HA) to obtain HA-SRF/Ce6@HANPs system. The designed nanoplatform destroys tumor cells in vitro and in vivo via the synergism of SRF (interrupting the exchange of cystine/glutamate by inhibiting SLC7A11) and photodynamic therapy (PDT, inducing reactive oxygen species generation). The decrease in tumor burden and reduction of extracellular glutamate significantly attenuate CIBP in mice model with developing bone cancer. Moreover, the combination of HA-SRF/Ce6@HANPs and PDT inhibit osteoclasts activation, promote osteoblast differentiation and accelerate bone repair. Overall, the nanoagent with good biocompatibility may provide an effective therapy method for the concurrent treatment of breast cancer bone metastasis and CIBP.
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