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  • Guangshan Xie, Lin Zhu, Yuanyuan Song, Wei Huang, Di Hu, Zongwei Cai
    Chinese Chemical Letters. 2021, 32(7): 2164-2168.

    Inflammation is a defense mechanism associated with a wide range of diseases. Celastrol is a small molecule isolated from traditional Chinese medicine with potent anti-inflammation activity. In this study, we established an integrated quantitative proteomics strategy to investigate the acute response to celastrol treatment in a rat macrophage cell line challenged with lipopolysaccharide (LPS). Both stable-isotopic based non-targeted quantitative profiling and PRM-based targeted quantitation methods were employed. Dimethyl-labeling based non-targeted profiling revealed 28 and 52 proteins that significantly up- and down-regulated by celastrol. Bioinformatics analysis pinpoint key signaling pathways affected. Seven proteins were selected for examining their time-dependent regulatory pattern in response to celastrol using targeted PRM quantitation. The abundance of mRNA at multiple time-points of selected proteins was also examined. Celastrol induced an acute response of selected key transcriptional factors in terms of mRNA or protein abundance within one hour. Interestingly, regulatory trend of mRNA and protein abundance suggested a novel dual mechanism of celastrol in the terms of acute anti-inflammation. The integrated quantitative proteomic strategy established in this study constitutes an efficient workflow to characterize key components and their time-dependent regulatory pattern for monitoring drug response.

  • Mei-Hua Shen, Ting-Biao Wan, Xiu-Rong Huang, Yan Li, Dan-Hua Qian, Hua-Dong Xu, Defeng Xu
    Chinese Chemical Letters. 2021, 32(7): 2297-2300.

    Borylative cyclization of E-3-arylallyl carbamoyl chlorides is achieved through copper catalyzed intramolecular carboboration with B2pin2. 2-Aryl-3-boryl-γ-lactams are formed with exclusive cis-diastereoselectivity. CuBr-Dppp combination gives the best outcomes. The substrate scope is profiled.

  • Zekun Xin, Xiaodong Zhao, Huiming Ji, Tianyi Ma, Hui Li, Shuhui Zhong, Zhurui Shen
    Chinese Chemical Letters. 2021, 32(7): 2151-2154.

    Carbon nanotube film (CNTF) can be used for photocatalysis and water treatment due to its porous structure, good stability and excellent electrical properties. In this work, TiO2/amorphous carbon/carbon nanotube film (TCC) composite with uniform structure was prepared by a simple atomization spraying method. Rhodamine B (RhB) was used to test the photocatalytic activity of TCC. TCC composite exhibits good photocatalytic activity under ultraviolet light. In particular, the degradation efficiency of rhodamine B (RhB) by TCC sprayed with 9 layers of TiO2 (9TCC) increased by 1.45 times than of TiO2 under ultraviolet light. The enhanced photocatalytic activity of TCC is attributed to the CNTF, which can broaden the light response range of TCC and improve the migration efficiency of electrons. The existence of amorphous carbon will promote these advances. Moreover, the better hydrophilic properties would enhance the catalytic performance happened on the solid-liquid interface. Finally, the photocatalytic mechanism and degradation intermediates of the TCC composite were proposed.

  • Guangze Nie, Shijun Qiu, Xiang Wang, Yan Du, Qingrui Zhang, Yang Zhang, Hengle Zhang
    Chinese Chemical Letters. 2021, 32(7): 2342-2346.

    Molybdenum disulfide (MoS2) has excellent trapping ability for lead ions whereas its micro-/nanoscale size has greatly impeded its practical applications in the flow-through systems. Herein, a millimeter-sized nanocomposite MoS2−001 was synthesized for Pb2+ removal by loading MoS2 nanosheets into a polystyrene cation exchanger D-001 by a facile hydrothermal method. The proposed structure and adsorption mechanism of MoS2−001 was confirmed by the scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) analysis. The nanocomposite showed outstanding adsorption capacity and rapid adsorption kinetic for Pb2+ removal, and the adsorption behavior followed the Langmuir adsorption model and pseudo-first-model kinetic model. Pb2+ uptake by MoS2−001 still maintains a high level even in the presence of extremely highly competitive ions (Ca(Ⅱ) and Mg(Ⅱ)), suggesting its high selectivity for Pb2+ adsorption. Besides, the fixed-bed column experiments further certified that MoS2−001 is of great potential for Pb2+ removal from the wastewater in practical engineering applications. Even more gratifying is that the exhausted MoS2−001 can be regenerated by NaCl-EDTANa2 solution without any significant adsorption capacity loss. Consequently, all the results indicated that MoS2−001 is a promising candidate adsorbent for lead-containing wastewater treatment.

  • Bo Zhen, Xinyue Suo, Jun Dang, Huilan Yue, Yanduo Tao, Jia-Jia Wang, Li Li, Ming-Bao Lin, Qi Hou, Wei-Ping Wang, Xiao-Liang Wang, Jian-Dong Jiang, Teng-Fei Ji
    Chinese Chemical Letters. 2021, 32(7): 2338-2341.

    Hyperterpenoid A (1) and B (2), two pairs of enantiomers, with an unprecedented 6/6/4/6/6 polycyclic skeleton, along with one known compoud hypermonone A (3) were isolated from Hypericum beanii. The racemate (±)-1 and (±)-2 were successfully separated into the two optically pure enantiomers (ee ≥ 99%) using a preparative HPLC system. Their absolute configurations were elucidated by extensive spectroscopic analyses and single-crystal X-ray diffraction method. The related plausible biogenetic pathways were presented. Compound 1-3 showed significant neuroprotective activity and potential anti-inflammatory activity. The result that (+)-2 and (-)-2 presented different anti-inflammatory properties, may lead us to new discovery of structure activity relationship between racemates, enantiomers, and diastereomers, as well as further research regarding the binding of drugs to target proteins.

  • Man Zhang, Weijian Wang, Xianhui Liang, Chang Li, Wenjun Deng, Haibiao Chen, Rui Li
    Chinese Chemical Letters. 2021, 32(7): 2217-2221.

    Aqueous supercapacitors (SCs) have attracted more and more attention for their safety, fast charge/discharge capability and ultra-long life. However, the application of aqueous SCs is limited by the low working voltage due to the narrow electrochemical stability window (ESW) of water. Herein, we report a new "water in salt" (WIS) electrolyte by dissolving potassium bis (fluorosulfonyl) amide (KFSI) in water with an ultra-high mass molar concentration of 37 mol/kg. The highly concentrated electrolyte can achieve a wide ESW of 2.8 V. The WIS electrolyte enables a safe carbon-based symmetrical supercapacitor to operate stably at 2.3 V with an ultra-long cycle life and excellent rate performance. The energy density reaches 20.5 Wh/kg at 2300 W/kg, and the capacity retention is 83.5% after 50, 000 cycles at a current density of 5 A/g. This new electrolyte will be a promising candidate for future high-voltage aqueous supercapacitors.

  • Liushan Jiang, Yu Xie, Fan He, Yun Ling, Jinsheng Zhao, Hao Ye, Shiqian Li, Jiangli Wang, Yang Hou
    Chinese Chemical Letters. 2021, 32(7): 2187-2191.

    A novel GO modified g-C3N4 nanosheets/flower-like BiOBr hybrid photocatalyst is fabricated by a facile method. The characterization results reveal that wrinkled GO is deposited between g-C3N4 nanosheets and flower-like BiOBr forming a Z-scheme heterojunction. As a mediator, plicate GO plays a positive role in prompting photogenerated electrons transferring through its sizeable 2D/2D contact surface area. The g-C3N4/GO/BiOBr hybrid displays a superior photocatalytic ability to g-C3N4 and BiOBr in photodegrading tetracycline (TC), whose removal efficiency could reach 96% within 2 h. Besides, g-C3N4/GO/BiOBr composite can reduce Cr(Ⅵ), and simultaneously treat TC and Cr(Ⅵ) combination contaminant under the visible light. The g-C3N4/GO/BiOBr ternary composite also exhibits satisfactory stability and reusability after four cycling experiments. Further, a feasible mechanism related to the photocatalytic process of g-C3N4/GO/BiOBr is put forward. This study offers a ternary hybrid photocatalyst with eco-friendliness and hopeful application in water pollution.

  • Wenqian Liu, Yulin Xu, Xue Li, Yan Meng, Huiling Wang, Chunrong Liu, Changlin Liu, Li Wang
    Chinese Chemical Letters. 2021, 32(7): 2322-2326.

    Nucleic acids with G4 elements play a role in the formation of aggregates involved in intracellular phase transitions. Our previous studies suggest that different forms of DNA could act as an accelerating template in Cu/Zn superoxide dismutase (SOD1) aggregation. Here, we examined the regulation of formation and cytotoxicity of the SOD1 aggregates by single-stranded 12-mer deoxynucleotide oligomers (dN)12 (N = A, T, G, C; ssDNAs) under acidic conditions. The ssDNAs can be divided into two groups based on their roles in SOD1 binding, exposure of hydrophobic clusters in SOD1, accelerated formation, morphology and cytotoxicity of SOD1 aggregates. G-quadruplexes convert SOD1 into fibrillar aggregates as a template, a fact which was observed for the first time in the nucleic acid regulation of protein aggregation. Moreover, the fibrillar or fibril-like SOD1 species with a G-quadruplex provided by (dG)12 were less toxic than the amorphous species with (dN)12 (N = A, T). This study not only indicates that both morphology and cytotoxicity of protein aggregates can be regulated by the protein-bound DNAs, but also help us understand roles of nucleic aid G-quadruplexes in the formation of aggregates and membraneless organelles involved in intracellular phase transitions.

  • Chenyi Yang, Shaoqing Zhang, Junzhen Ren, Pengqing Bi, Xiaotao Yuan, Jianhui Hou
    Chinese Chemical Letters. 2021, 32(7): 2274-2278.

    The power conversion efficiencies (PCEs) of organic solar cells (OSCs) have reached 18% recently, which have already met the demand of practical application. However, these outstanding results were generally achieved with donor-acceptor (D-A) type copolymer donors, which can hardly fulfill the low-cost large-scale production due to their complicated synthesis processes. Therefore, developing polymer donors with simple chemical structures is urgent for realizing low-cost OSCs. Polythiophene (PT) derivatives are currently regarded as promising candidates for such kind of donor materials, which has been illustrated in many works. In this work, two new alkylthio substituted PT derivatives, P301 and P302, were synthesized and tested as donors in the OSCs using Y5 as the acceptor. In comparison, the introduction of fluorine atoms on the backbone of P302 can not only downshift the energy levels, but also greatly improve the phase separation morphologies of the active layers, which is ascribed to the enhanced aggregation effect and the reduced miscibility with the non-fullerene acceptor. As a result, the P302:Y5-based OSC exhibits a significantly improved PCE of 9.65% than that of P301:Y5-based one, indicating the important role of fluorination in the construction of efficient PT derivative donors.

  • Meiling Shui, Chao Huang, Peiyu Ma, Wenjie Li, Qun He, Wenlong Wu, Yisheng Tan, Jun Bao
    Chinese Chemical Letters. 2021, 32(7): 2203-2206.

    With regard to the reaction of higher alcohol synthesis (HAS), the optimizations of activity and selectivity towards C2+ alcohol are restricted by the improper equilibrium in two different CO activation pathways and chain growth capacity. Herein, we find that delibrately controlling the compositions of catalysts is an effective strategy to achieve the equilibrium of CO activation pathways and promote the chain growth. As a result, the optimized Cu0.25Co0.75 alloy catalyst can achieve a large proportion of higher alcohol in alcohol products (C2+OH/MeOH = 4.40), together with high CO conversion of 71.27% and space-time-yield of 147.65 g kg−1 h−1. The mechanistic studies suggest that the good performance of Cu0.25Co0.75 catalyst is attributed to the synergistic effect between alloyed Cu and Co.

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