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1.
Covalent organic frameworks(COFs) are emerging photocatalysts for hydrogen evolution in water splitting in recent years. They offer a pre-designable platform to design tailor-made structures and chemically adjustable functionality in terms of photocatalysis. In this review, we summarize the recent striking progress of COF-based photocatalysts in design and synthesis. Firstly, different approaches to functionalizing building blocks, diversifying linkages, extending π-conjugation and establishing D-A conjugation are illustrated for enhancing photocatalytic activity. Next, post-modification of backbones and pores is detailed for emphasizing the synergistic catalytic uniqueness of COFs. Besides, the strategy of preparing COF-related composites with various semiconductors is outlined for optimizing the electronic properties. Finally, we conclude with the current challenges and promising opportunities for the exploration of new COF-based photocatalysts. 相似文献
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《中国化学快报》2022,33(4):1889-1894
Permeation enhancers (PEs), such as N-[8-(2-hydroxybenzoyl)amino]-caprylate (SNAC), have been reported to improve the oral absorption of various macromolecules. However, the bioavailabilities of these formulations are quite low and variable due to the influences of enzymes, pH and other gastrointestinal barriers. In this study, we revealed that SNAC could interact with insulin to form tight complexes in a specific concentration (insulin ≥ 40 µg/mL)-, ratio (SNAC/insulin ≥ 20:1)- and pH (≥ 6.8)-dependent manner, thus contributing to a significantly high efficacy of oral insulin delivery. Specifically, absorption mechanism studies revealed that the SNAC/insulin complexes were internalized into the cells by passive diffusion and remained intact when transported in the cytosol. Furthermore, the complexes accelerated the exocytosis of insulin to the basolateral side, thereby enhancing its intestinal mucosal permeability. Eudragit? S100-entrapped SNAC/insulin microspheres were then prepared and exhibited an apparent permeability coefficient (Papp) that was 6.6-fold higher than that of the insulin solution. In diabetic rats, hypoglycemic activity was sustained for more than 10 h after the microspheres were loaded into enteric-coated capsules. Further pharmacokinetic studies revealed an approximately 6.3% oral bioavailability in both the fasted and fed states, indicating a negligible food effect. Collectively, this study provides insight into the interaction between PEs and payloads and presents an SNAC-based oral insulin delivery system that has high oral bioavailability and patient-friendly medication guidance. 相似文献
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《中国化学快报》2020,31(6):1593-1597
As one of the most environmentally friendly photovoltaic(PV) conversion equipments,aqueousprocessed CdTe nanocrystal solar cells(NC SCs) have attracted great interest in recent years because of their excellent properties such as high charge-carrier mobility and broad absorption.However,two issues including interfacial recombination and leakage current seriously restrict their performance.In this paper,insulating polymer poly(vinyl pyrrolidone)(PVP) is introduced into CdTe NC SCs to solve the problems.The experimental results of transmission electron microscopy(TEM),atomic force micro scopy(AFM) and dark current measurements,etc.,demonstrate the leakage current is effectively suppressed by introducing PVP.Through further designing device structure,the reduction of interfacial recombination after introducing PVP is confirmed.By strategically taking the advantages of PVP properties(e.g.,water solubility and thermostability),the power conversion efficiency of the devices with PVP is enhanced by almost 37% compared to pure CdTe devices.This work demonstrates an effective and low-cost method to fabricate NC SCs via aqueous route.Moreover,it also proves that appropriate content of insulating polymer is of beneficial in promoting the PV performance. 相似文献
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《中国化学快报》2020,31(7):1782-1786
Anodic electrocatalyst plays the core role in direct alcohol fuel cells (DAFCs), while traditional Pt-catalysts suffer from limited catalytic activity, high over potential and severe CO poisoning. Herein, by selectively depositing Rh atoms on the defective-sites of Pt nanowires (NWs), we developed a new Pt@Rh NW electrocatalyst that exhibited enhanced electrocatalytic performance for both methanol oxidation (MOR) and ethanol oxidation (EOR). Both cyclic voltammetry (CV) and in-situ infrared spectroscopy revealed that the presence of Rh atoms suppressed the generation of poisonous intermediates and completely oxidized alcohols molecule into CO2. Atomic resolusion spherical aberration corrected high-angle annular dark field scanning transmission electron microscopy (CS-HAADF-STEM) and energy-dispersive X-ray spectroscopy (EDS) mapping analysis revealed that Rh atoms were primarily deposited on the defective sites of Pt NWs. Meanwhile, the presence of Rh atoms also modified the electronic state of Pt atoms and therefore lowered the onset potential for alcohols oxidation potential. This work gives the first clear clue on the role of the defective sites of Pt nanocatalyst poisoning, and propose that selectively blocking these sites with trace amount of Rh is an effective strategy in designing advantageous electrocatalysts. 相似文献
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Shuangshuang Ji Xiuzhu Yang Xiaolong Chen Ang Li Doudou Yan Haiyan Xu Hao Fei 《Chemical science》2020,11(34):9126
The development of chemotherapy, an important cancer treatment modality, is hindered by the frequently found drug-resistance phenomenon. Meanwhile, researchers have been enthused lately by the synergistic use of chemotherapy with emerging immunotherapeutic treatments. In an effort to address both of the two unmet needs, reported herein is a study on a series of membrane active iridium(iii) complexed oligoarginine peptides with a new cell death mechanism capable of overcoming drug resistance as well as stimulating immunological responses. A systematic structure–activity relationship study elucidated the interdependent effects of three structural factors, i.e., hydrophobicity, topology and cationicity, on the regulation of the cytotoxicity of the Ir(iii)-oligoarginine peptides. With the most prominent toxicities, Ir-complexed octaarginines (R8) were found to display a progressive oncotic cell death featuring cell membrane-penetration and eruptive cytoplasmic content release. Consequently, this membrane-centric death mechanism showed promising potential in overcoming multiple chemical drug-resistance of cancer cells. More interestingly, the eruptive mode of cell death proved to be immunogenic by stimulating the dendritic cell maturation and inflammatory factor accumulation in mice tumours. Taking these mechanisms together, this work demonstrates that membrane active compounds may become the next generation chemotherapeutics because of their combined advantages.Structure optimized Ir-complexed cyclic octa-arginine shows a potential of “one-drug two-effects” for cancer treatment. 相似文献
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Ping Chen Yanhong Hao Xinxin Wang Prof. Dr. Dan Yuan Prof. Dr. Yingming Yao Prof. Dr. Lutz Ackermann 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(30):7292-7297
Highly position selective alkylations of N-alkylindoles at C7-positions have been enabled by cationic zirconium complexes. The strategy provides a straightforward access to install alkyl groups at C7-positions of indoles without a complex directing group. Mechanistic studies provided support for the importance of Brønsted acids in the catalytic manifold. 相似文献
10.
Wu Tong Dr. Qi Shao Pengtang Wang Prof. Xiaoqing Huang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(29):7218-7224
The design and development of non-noble metal alternatives with superior performance and promising long-term stability that is comparable or even better than those of noble-metal-based catalysts is a significant challenge. Here, we report the thermal-induced phase engineering of non-noble-metal-based nanowires with superior electrochemical activity and stability for the methanol oxidation reaction (MOR) under alkaline conditions. The optimized Cu–Ni nanowires deliver an unprecedented mass activity of 425 mA mg−1, which is 4.3 times higher than that of the untreated one. Detailed catalytic investigations show that the enhanced performance is due to the large active area, the increased number of active sites (NiOOH), and fast methanol electrooxidation kinetics. In addition, the generated hollow feature in the nanowires provides a unique void space to release the volume expansion, where the activity can be maintained for 5 h without a distinct activity decay. The present work emphasizes the importance of precisely phase modulating of nanomaterials for the design of non-noble metal electrocatalysts towards the MOR, which opens up a new pathway for the design of cost-effective electrocatalysts with promising activity and long-term stability. 相似文献