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  • Hangqi Zhu, Bing Zhang, Nali Zhu, Mingchun Li, Qilin Yu
    Chinese Chemical Letters. 2021, 32(3): 1220-1223.

    In this study, we prepared mitochondrion targeting peptide-grafted magnetic graphene oxide (GO) nanocarriers for efficient impairment of the tumor mitochondria. The two-dimensional GOMNP-MitP nanosheets were synthesized by grafting magnetic γ-Fe2O3 to the surface of GO, followed by covalent modification of mitochondrion targeting peptide (MitP). GOMNP-MitP exhibited the high capacity of loading the anticancer drug mitoxantrone (MTX), and preferentially targeted the tumor mitochondria. With the aid of alternating magnetic field (AMF), the MTX-loading GOMNP-MitP released MTX to the mitochondria, severely impairing mitochondrial functions, including attenuation of ATP production, decrease in mitochondrial membrane potential (MMP), and further leading to activation of apoptosis. This study realized high-efficient mitochondrion-targeting drug delivery for anticancer therapy by two-dimensional nanoplatforms.

  • Xiao-Feng He, Ji-Jun Chen, Tian-Ze Li, Jing Hu, Xu-Ke Zhang, Yuan-Qiang Guo, Xue-Mei Zhang, Chang-An Geng
    Chinese Chemical Letters. 2021, 32(3): 1202-1205.

    Tsaokols A (1) and B (2), two complicated flavanol-monoterpenoid hybrids, were isolated from the dried fruits of Amomum tsao-ko under the guidance of LCMS and bioassay. Their structures were determined by extensive spectroscopic analyses and electronic circular dichroism (ECD) calculations. Compounds 1 and 2 shared a flavanol backbone fused with 5/7 and 5/6 bicyclic monoterpenoid scaffolds, which were biogenetically condensed by Michael addition and acetalization. Compounds 1 and 2 exhibited significant α-glucosidase inhibitory activity with IC50 values of 18.8 and 38.6 μmol/L (acarbose, IC50 = 213 μmol/L). Docking study supported the strong interactions of 1 and 2 bonding with enzyme by mainly hydrophobic and hydrogen-bond effects. Compounds 1 and 2 could be fast distinguished by the diagnostic ions at m/z 289 and 313 in negative MS2 experiments.

  • Xueying Lu, Yajing Sun, Zhicheng Zhang, Zhigang Shuai, Wenping Hu
    Chinese Chemical Letters. 2021, 32(3): 1233-1236.

    High-mobility and strong luminescent materials are essential as an important component of organic photodiodes, having received extensive attention in the field of organic optoelectronics. Beyond the conventional chemical synthesis of new molecules, pressure technology, as a flexible and efficient method, can tune the electronic and optical properties reversibly. However, the mechanism in organic materials has not been systematically revealed. Here, we theoretically predicted the pressure-depended luminescence and charge transport properties of high-performance organic optoelectronic semiconductors, 2, 6-diphenylanthracene (DPA), by first-principle and multi-scale theoretical calculation methods. The dispersion-corrected density functional theory (DFT-D) and hybrid quantum mechanics/molecular mechanics (QM/MM) method were used to get the electronic structures and vibration properties under pressure. Furthermore, the charge transport and luminescence properties were calculated with the quantum tunneling method and thermal vibration correlation function. We found that the pressure could significantly improve the charge transport performance of the DPA single crystal. When the applied pressure increased to 1.86GPa, the hole mobility could be doubled. At the same time, due to the weak exciton coupling effect and the rigid flat structure, there is neither fluorescence quenching nor obvious emission enhancement phenomenon. The DPA single crystal possesses a slightly higher fluorescence quantum yield ~ 0.47 under pressure. Our work systematically explored the pressure-dependence photoelectric properties and explained the inside mechanism. Also, we proposed that the external pressure would be an effective way to improve the photoelectric performance of organic semiconductors.

  • Pengbo Ye, Xuan Liu, Gang Wang, Lei Liu
    Chinese Chemical Letters. 2021, 32(3): 1237-1240.

    A nickel(Ⅱ)-catalyzed asymmetric alkylation of acyclic oxocarbenium ions generated in situ from corresponding acetals with carboxylic acid derivatives to prepare β-alkoxyl carbonyl moieties with diverse α-substituents has been disclosed. The method exhibited broad scope of acetals and carboxylic acid derivatives with excellent enantioselectivity and good functional group compatibility, and can be conducted in a gram-scale without obvious loss of efficiency.

  • Qin Li, Jin Niu, Meiling Dou, Zhengping Zhang, Feng Wang
    Chinese Chemical Letters. 2021, 32(3): 1181-1185.

    Non-enzymatic electrochemical sensors for the determination of hydrogen peroxide (H2O2) have attracted more and more concerns. A series of nickel and cobalt double oxides (NixCoy-DO) with the different ratios of Ni/Co have been prepared by a polyol-mediated solvothermal method for H2O2 detection. The obtained products exhibit honeycomb-like open porous microtubes constituted with the low-dimensional nanostructured NixCoy-DO blocks after the calcination treatment. Compared with nickel oxides, the introduced Co ions in NixCoy-DO can induce the production of surficial oxygen vacancies, and further enhance the electrode surface activity. In particular, the NiCo-DO sample (with an atomic ratio of Ni/Co = 4:3) shows the richest surficial oxygen vacancies and presents the highest H2O2 detection activity among all the as-prepared samples, demonstrating an excellent sensitivity of 698.60 μA L mmol-1 cm-2 (0 ~ 0.4 mmol/L), low detection limit (0.28 μmol/L, S/N = 3), as well as long stability, high selectivity and good reproducibility. This work lends a new impetus to the potential application of double metal oxides for the next generation of non-enzymatic sensors.

  • Chen Yan, Jing Sun, Chao-Guo Yan
    Chinese Chemical Letters. 2021, 32(3): 1253-1256.

    p-TsOH catalyzed Diels-Alder reaction of 3-(indol-3-yl)maleimides with 3-phenacylideneoxindoles in toluene at 80 ℃ for two hours afforded cis/trans isomers of 3a', 4′, 6′, 10c'-tetrahydrospiro[indoline-3, 5′-pyrrolo[3, 4-c]carbazoles] in nearly comparable yields, which could be easily converted to the corresponding 4′, 6′-dihydrospiro[indoline-3, 5′-pyrrolo[3, 4-c]carbazole] in high yields and with high diastereoselectivity by further DDQ oxidation., the similar reaction of 3-(indol-3-yl)maAdditionallyleimides with 2-arylidene-1, 3-indanediones in toluene 80 ℃ and sequential DDQ oxidation afforded functionalized dihydrospiro[indene-2, 5′-pyrrolo[3, 4-c]carbazoles] as major products.

  • Tao Wang, Juan Du, Yong Sun, Xing Tang, Zuo-Jun Wei, Xianhai Zeng, Shi-Jie Liu, Lu Lin
    Chinese Chemical Letters. 2021, 32(3): 1186-1190.

    Catalytic transfer hydrogenation (CTH) of furfural (FF) to furfuryl alcohol (FFA) has received great interest in recent years. Herein, Cu-Cs bimetallic supported catalyst, CuCs(2)-MCM, was developed for the CTH of FF to FFA using formic as hydrogen donor. CuCs(2)-MCM achieved a 99.6% FFA yield at an optimized reaction conditions of 170 ℃, 1 h. Cu species in CuCs(2)-MCM had dual functions in catalytically decomposing formic acid to generate hydrogen and hydrogenating FF to FFA. The doping of Cs made the size of Cu particles smaller and improved the dispersion of the Cu active sites. Importantly, the Cs species played a favorable role in enhancing the hydrogenation activity as a promoter by adjusting the surface acidity of Cu species to an appropriate level. Correlation analysis showed that surface acidity is the primary factor to affect the catalytic activity of CuCs(2)-MCM.

  • Tian Bai, Kongyin Zhao, Zijie Lu, Xuefang Liu, Ze Lin, Mengmeng Cheng, Ziyi Li, Dunwan Zhu, Linhua Zhang
    Chinese Chemical Letters. 2021, 32(3): 1051-1054.

    Herein, copper ion doped calcium alginate (Cu2+/CaAlg) composite hydrogel filtration membranes were prepared by using natural polymer sodium alginate (NaAlg) as raw material. The thermal stability and structure of the composite membranes were characterized by thermogravimetric analysis and infrared spectroscopy. The mechanical strength, anti-fouling performance, hydrophilicity and filtration performance of the membrane were studied. The results show that Cu2+/CaAlg hydrogel membrane has excellent mechanical properties and thermal stability. The anti-swelling ability of the membrane was greatly enhanced by doping Cu2+. After three alternate filtration cycles, the flux recovery rate of Cu2+/CaAlg hydrogel membrane can still reach 85%, indicating that the membrane has good anti-pollution performance. When the operation pressure was 0.1 MPa, the rejection of coomassie brilliant blue G250 reached 99.8% with a flux of 46.3 L m-2 h-1, while the Na2SO4 rejectionwas less than 10.0%. The Cu2+/CaAlg membrane was recycled after 24 h in the filtration process, and its flux and rejection rate did not decrease significantly, indicating that the hydrogel membrane has long-term application potential. The Cu2+/CaAlg membrane has a wide range of applications prospect in dye desalination, fine separation and biopharmaceutical technology fields.

  • Pu Shi, Xiaodi Cheng, Siliu Lyu
    Chinese Chemical Letters. 2021, 32(3): 1210-1214.

    Developing highly efficient nickel or iron based hydroxide electrocatalysts is primary essential but challenging for oxygen evolution reaction (OER) at ultra-high current densities. Herein, we developed a facile method to prepare nitrogen and iron doped nickel(Ⅱ) hydroxide nanosheets on self-supported conductive nickel foam (denoted as Fe, N-Ni(OH)2/NF) through ammonia hydrothermal and impregnation methods. Owing to the optimization of the electronic structure by nitrogen doping and the strong synergistic effect between Fe and Ni(OH)2, the three-dimensional (3D) Fe, N-Ni(OH)2/NF nanosheets delivered superior electrocatalytic OER performances in basic solution with low potentials of 1.57V and 1.59V under 500mA/cm2 and 1000mA/cm2 respectively and robust operation for 10 h with ignored activity decay, comparing well with the potentials of previously reported NiFe based electrocatalysts as well as the benchmark commercial Ir/C/NF. In-situ Raman spectroscopy revealed that the main active species were NiOOH during the OER process. The present results are expected to provide new insights into the study of OER process towards ultra-high current densities.

  • Xiaokang Wang, Yutong Wang, Kebin Lu, Weifeng Jiang, Fangna Dai
    Chinese Chemical Letters. 2021, 32(3): 1169-1172.

    An unexpected in-situ hydrolysis reaction occurred during the solvothermal reaction of N, N'-bis(4-carboxy-2-methylphenyl)pyromellitic di-imide) and Ba(NO3)2, and a novel porous Ba-MOF, [H2N(CH3)2]0.5[Ba1.5(L)(DMA)]·1.5DMA·1.5H2O (UPC-70, H3L = 2-(4-carboxy-2-methylphenyl)-1, 3-dioxoisoin-doline-5, 6-dicarboxylic acid, DMA = N, N-dimethylacetamide), was obtained on the basis of the partial hydrolysate. The as-synthesized 3D network with 1D open channels of different sizes (24 Å and 10 Å) contains abundant open metal sites after removal of solvents, which is conducive to the preferential adsorption of CO2. The subsequent gas sorption measurement reveals the high separation selectivity of UPC-70 for CO2/CH4 (15) and CO2/N2 (32) at ambient conditions, and GCMC theoretical simulation provides good verification of the experimental results, indicating that UPC-70 is a potential candidate for CO2 capture from flue gas and natural gas.

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