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  • Jinrong Zheng, Shuheng Qin, Lijuan Gui, Hua Li, Lixue Fan, Yifei Yang, Haiyan Chen, Hui Xu, Zhenwei Yuan
    Chinese Chemical Letters. 2021, 32(8): 2385-2389.

    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.

  • Mengdi Sun, Zemin Zhang, Qiujin Shi, Jianlong Yang, Mingzheng Xie, Weihua Han
    Chinese Chemical Letters. 2021, 32(8): 2419-2422.

    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.

  • Xinfu Zhang, Lu Wang, Ning Li, Yi Xiao
    Chinese Chemical Letters. 2021, 32(8): 2395-2399.

    Here we propose a fluorescent sensor, Chroma-V, consisted of a Hoechst ligand (Hoe) to target chromatin DNA and a BODIPY rotor (BDP) to sense the local viscosity that reflects chromatin condensation state. Within Chroma-V, efficient FRET process from Hoe to BDP facilitated a single-excitation ratiometric imaging of nucleus DNA under fluorescence confocal microscope, which utilized the ratio of two channels to enable an intuitive visualization of chromatin condensation state. And fluorescence lifetime imaging (FLIM) based on fluorescent signal from BDP proved to be a more accurate method to quantify the changes of chromatin condensation state under different epigenetic states, including histone acetylation regulated by deacetylase inhibitors, cell apoptosis induced by DNA-bining drugs, and the epithelial-mesenchymal transition of HUVEC cells induced by TGF-β.

  • Dongxu Yang, Jialiang Liang, Liang Luo, Ruoyu Deng, Guo Li, Qiang He, Yi Chen
    Chinese Chemical Letters. 2021, 32(8): 2534-2538.

    Semiconductor-mediated photocatalysis is a promising photochemical process for harvesting inexhaustible solar energy to address the energy crisis and environmental issues. However, the low solar-light response and poor carrier migration are severe drawbacks that limit its practical application. Herein, we propose a convenient pathway for improving electron-hole separation and solar energy utilisation by engineering defective ZnIn2S4 with doping of carbon dots. The optimum ZnIn2S4/CD200 nanosheet exhibited 100% diclofenac (DCF) degradation within 12 min under visible-light. The estimated photocatalytic efficiency under natural sunlight was 98.2%. Scavenging experiments and electron spin resonance (ESR) analysis indicated that the superoxide radical (O2), photoelectron (e), hole (h+) and hydroxyl radical (OH) were the predominant contributions in the ZnIn2S4/CD200/DCF/visible light system. Furthermore, ZnIn2S4/CD200 exhibited excellent reusability and stability after 4 times recycling. The photodegradation routes mainly involved hydroxylation, decarboxylation, CN bond cleavage, dechlorination, ring closure, and ring-opening. The ecological risk assessment and total organic carbon (TOC) tests exhibited desirable toxicity reduction and mineralization results. These observations not only offer a facile strategy for the construction of defective ZnIn2S4, but also pioneer the direct utilisation of natural light for highly efficient environmental remediation.

  • Jialiang Wei, Jie Li, Chuang Yu, Qimeng Sun, Jinghui He, Jianmei Lu
    Chinese Chemical Letters. 2021, 32(8): 2463-2468.

    Ion-in-conjugation (IIC) materials are emerging as an important class of organic electronic materials with wide applications in energy storage, resistive memories and gas sensors. Many IIC materials were designed and investigated, however the role of conjugation in IIC materials' performance is yet investigated. Here we designed two molecules obtained by condensation of 4-butylaniline and oxocarbon acid. Squaric acid derivatives squaraine named SA-Bu and a croconamide named CA-Bu which only differ in their oxocarbon cores. While employing SA-Bu and CA-Bu as resistive memory and gas sensory materials, SA-Bu has attained promising performance in ternary memory and detection of NO2 as low as 10 parts-per-billion whereas CA-Bu show mainly binary memory behavior and negligible NO2 response. Theoretical calculations reveal that conjugation of CA-Bu was distorted by the increased steric hindrance, frustrating the charge transport and suppressing the conductivity. Our work demonstrates that the conjugation plays a crucial role in ion-in-materials promoting ternary RRAM devices and high-performance gas sensors manufacture.

  • Zhishu Zeng, Yunqian Zhang, Xiaodong Zhang, Guangyan Luo, Jun Xie, Zhu Tao, Qianjun Zhang
    Chinese Chemical Letters. 2021, 32(8): 2572-2576.

    In this paper, the host-guest interaction of cucurbit[7]uril (Q[7]) and chromone (CMO) has been developed as a fluorescent probe for the highly selective detection of Zn2+ and Cd2+ in water based on a chelation-enhanced fluorescence (CHEF) mechanism. There was a good linear relationship between the fluorescence intensity of the CMO@Q[7] probe and the concentration of Zn2+ or Cd2+ in the range of 0–3.0 × 10–5 mol/L and the detection limit for Zn2+ and Cd2+ was found to be 2.03 × 10–6 mol/L and 1.89 × 10–6 mol/L, respectively. The X-ray crystal structure indicated that different coordination fashions were triggered by Zn2+ and Cd2+ in the CMO@Q[7] complexes, respectively. However, both metal ions coordinated with the carbonyl oxygen of CMO, which was encapsulated in the cavity of Q[7], thus leading to the enhancement of recognition fluorescence emission of CMO.

  • Zhonghua Qu, Pu Wang, Xing Chen, Guo-Jun Deng, Huawen Huang
    Chinese Chemical Letters. 2021, 32(8): 2582-2586.

    Visible-light-driven photochemical Cadogan-type cyclization has been discovered. The organic D-A type photosensitizer 4CzIPN found to be an efficient mediator to transfer energy from photons to the transient intermediate that breaks the barriers of deoxygenation in Cadogan reaction and enables a mild metal-free access to carbazoles and related heterocycles. DFT calculation results indicate mildly endergonic formation of the intermediate complex of nitrobiarenes and PPh3, which corresponds with experimental findings regarding reaction temperature. The robust synthetic capacity of the photoredox Cadogan reaction systems has been demonstrated by the viable productivity of a broad range of carbazoles and related N-heterocycles with good tolerance of various functionalities.

  • Jiaqiang Wu, Yanfang Liu, Xuejing Yang, Jinling Wang, Jie Yang
    Chinese Chemical Letters. 2021, 32(8): 2503-2508.

    The textile industry spreads globally with the challenges of its wastewater treatment, especially dyes, which are difficult to degrade. To improve coagulation-flocculation process in dye wastewater treatment, an intercalation process was employed to prepare a new efficient coagulant of lithium borohydride-iron oxychloride (LiBH4_FeOCl) in this study. The layered crystal pristine iron oxychloride (FeOCl) material was prepared by chemical gas phase migration. LiBH4 was introduced into the layers of two dimensional (2D) FeOCl nanosheets by a simple method of liquid phase insertion. The samples were characterized by a field emitting scanning electron microscopy (SEM), a rotating anode X-ray powder diffractometer (XRD), etc. The cationic dye was employed as the simulated pollutant. A coagulation and decolorization experimental device was built to study the coagulation performance of the new coagulant LiBH4_FeOCl. It is found that the intercalation modified LiBH4_FeOCl exhibits the characteristics of crystal structure, and the layered structure of FeOCl is preserved. LiBH4_FeOCl, as an insoluble inorganic solid coagulant, performs well for dye pollutants of methyl red, basic yellow 1, methylene blue, rhodamine B, ethyl violet and Janus green B. The reaction rate is significantly 68% higher than the current commercial coagulants of Al2(SO4)3. The mechanism analysis reveals that LiBH4_FeOCl breaks and disperses rapidly in the water environment. Its negatively charged material particles can be electrostatically adsorbed with dye pollutant molecules through electrostatic action. The above collaborative actions of breaking, dispersion and electrostatic adsorption are the main coagulation mechanisms of LiBH4_FeOCl. The solid inorganic coagulant of LiBH4_FeOCl provides a competitive alternative for traditional inorganic salts and organic coagulants.

  • Changwei Chen, Hongyu Zhang, Gang Xu, Sunliang Cui
    Chinese Chemical Letters. 2021, 32(8): 2551-2554.

    Ynamides are electron-rich alkynes with unique reactivities and act as flexible building blocks in organic synthesis. Therefore, the investigation for transformation of ynamides with exceptional selectivity and efficiency is attractive and interesting. Herein, we report an oxoarylation of ynamides with N-aryl hydroxamic acids. In the presence of catalytic Cu(OTf)2, both the terminal and internal ynamides could undergo an addition/[3,3] sigmatropic rearrangement cascade with N-aryl hydroxamic acids to achieve oxoarylation, along with providing selective entry to (ortho-amino)arylacetamides and oxindoles. Moreover, deuterium-labelling reaction and gram-scale reaction were conducted to probe the mechanism and showcase the scalability.

  • Pengjia Ding, Jianrui Niu, Fengqin Chang, Zhuang He, Thomas Wågberg, Zaixing Li, Guangzhi Hu
    Chinese Chemical Letters. 2021, 32(8): 2495-2498.

    Morphology and dispersity are key factors for activating peroxymonosulfate (PMS). In this study, we designed a recyclable open-type NiCo2O4 hollow microsphere via a simple hydrothermal method with the assistance of an NH3 vesicle. The physical structure and chemical properties were characterized using techniques such as scanning electron microscope (SEM), transmission electron microscope (TEM), X-ray diffraction (XRD), N2 adsorption and X-ray photoelectron spectroscopy (XPS). The test results confirm that the inner and outer surfaces of open-type NiCo2O4 hollow-sphere can be efficiently utilized because of the hole on the surface of the catalyst, which can minimize the diffusion resistance of the reactants and products. Under optimized conditions, the total organic carbon (TOC) removal efficiency of rhodamine B (RhB) can reach up to 80% in 40 min, which is almost 50% shorter than the reported values. The reactive radicals were identified and the proposed reaction mechanism was well described. Moreover, the disturbances of HCO3, NO3, Cl and H2PO4 were further investigated. As a result, HCO3 and NO3 suppressed the reaction while Cl and H2PO4 had a double effect on reaction.

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