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  • Han Zhang, Yingchao Lin, Zhengyu Men, Masaru Ihara, Weizun Li, Kai He
    Chinese Chemical Letters. 2020, 31(10): 2859-2863.

    The occurrence of biologically active pharmaceuticals in aquatic environments raised the potential risks to aquatic species. Among these marketed biological active pharmaceuticals, it has been estimated that 40% of them target G-protein-coupled receptors (GPCRs). We have illustrated pharmaceutical activities of GPCR targeted pharmaceuticals in English and Japanese wastewater by the in vitro transforming growth factor-α (TGFα) shedding assay. However, as the most important producer and consumer of pharmaceuticals, the occurrence of GPCR targeted pharmaceuticals in China had remained unclear. In this study, we investigated the pharmaceutical activities of GPCR targeted pharmaceuticals in secondary effluents of Chinese wastewater treatment plants. We discovered antagonistic activities against angiotensin (AT1) receptor at up to 7.2×102 ng-valsartan-equivalent quantity/L in Chinese wastewater for the first time as well as agonistic activities against dopamine (D2) receptor. Furthermore, in parallel with the assay, we determined concentrations of GPCR targeted pharmaceuticals in target wastewater by liquid chromatography coupled with tandem mass spectrometry (LC–MS/MS). Through the comparison of predicted antagonistic activities calculated by concentrations and potency values from the assay, we found that the measured antagonistic activities against AT1 receptor from the assay were higher than the predicted AT1 activities from valsartan, irbesartan, and losartan, indicating the potential existence of other unknown AT1 antagonists in wastewater.

  • Zhaoyang Wang, Xiaolei Teng, Mingzheng Xie, Xiuwen Cheng, Junfeng Li
    Chinese Chemical Letters. 2020, 31(10): 2864-2870.

    In this study, various conditions for the removal of polyvinyl alcohol (PVA) by electrocoagulation (EC) coupled catalytic oxidation are systematically studied. The direct oxidation of the anode, the reduction of the cathode, the oxidation of ·OH and ·Cl, and the synergistic effect of flocculation on the degradation of polyvinyl alcohol are investigated. It is observed that the optimum experimental conditions obtained are as follows: Cell voltage 9 V, natural pH 7, NaCl concentration 0.02 mol/L, and interelectrode distance 3.0 cm. The evolution of iron ions is also discussed in the EC process. By contrast, EC had made an outstanding contribution to the removal of PVA, which removes 71.29% of PVA. Free radicals, especially ·OH and ·Cl, are equivalent to the contribution of the electrodes in the degradation of PVA. And the contribution of PVA degradation by anode oxidation and cathode reduction are 12.76% and 8.02%, respectively. Characterization of solution and floc, such as Fourier transform infrared spectrometry (FTIR), scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS), thermogravimetric analysis (TGA), GC–MS and molecular weight, showed that PVA is effectively removed by the EC process, and a possible degradation pathway is proposed.

  • Liming Peng, Yucui Bian, Xiaoqing Shen, Hong-Chang Yao, Haijun Chen, Zhongjun Li
    Chinese Chemical Letters. 2020, 31(10): 2871-2875.

    Metal nanoclusters have shown great potential in photocatalysis, while simultaneous removal of both inorganic and organic contaminants by metal nanoclusters under visible light is less explored. Here, we synthesized Agm(SR)n (SR represents 3-mercaptopropyltriethoxysilane ligand) nanoclusters (~1 nm) via a reduction of silver triphenylphosphine under ambient conditions in the presence of 3-mercaptopropyltriethoxysilane. The nanocluster was characterized by UV–vis spectroscopy, high resolution transmission electron microscopy (HRTEM), Fourier transform infrared spectrum (FTIR), and X-ray photoelectron spectroscopy (XPS). Under 5 W blue LED, the Agm(SR)n/P25 exhibits enhanced catalytic activity for simultaneous methyl orange (MO) oxidation and Cr(Ⅵ) reduction, and also for synchronous 4-chlorophenol oxidation and Cr(Ⅵ) reduction. Mechanism studies by electrochemical impedance spectroscopy (EIS), photoluminescence (PL), electron spin resonance (ESR) etc. and control experiments reveal that the unique structure of silver nanoclusters with thiolate ligands is vital to the high catalytic performance, and both the photo-generated holes and superoxide radicals are responsible for the decomposition of MO.

  • Zhengtong Li, Chengbing Wang
    Chinese Chemical Letters. 2020, 31(9): 2159-2166.

    Access to safe drinking water has become an extremely urgent research topic worldwide. In recent years, the technology of solar vapor generation has been extensively explored as a potential and effective strategy of transforming elements content in seawater. In this review, the basic concepts and theories of metal-based photothermal vapor generation device (PVGD) with excellent optical and thermal regulatory are introduced. In the view of optical regulation, how to achieve high-efficiency localized evaporation in different evaporation system (i.e., volumetric solar heating and interface solar heating) is discussed; from the aspect of thermal regulation, the importance of selective absorption surface for interfacial PVGD is analyzed. Based on the above discussion and analysis, we summarize the challenges of metal-based desalination device.

  • Qi Wang, Shiyong Chu, Shaohua Guo
    Chinese Chemical Letters. 2020, 31(9): 2167-2176.

    As one of the most promising secondary batteries in large-scale energy storage, sodium ion batteries (SIBs) have attracted wide attention due to the abundant raw materials and low cost. Layered transition metal oxides are one kind of popular cathode material candidates because of its easy synthesis and large theoretical specific capacity. Yet, the most common P2 and O3 phases show distinct structural characteristics respectively. O3 phase can serve as a sodium reservoir, but it usually suffers from serious phase transition and sluggish kinetics. For the P2 phase, it allows the fast sodium ion migration in the bulk and the structure can maintain stable, but it is lack of sodium, showing a great negative effect on Coulombic efficiency in full cell. Thus, single phase structure almost cannot achieve satisfied comprehensive sodium storage performances. Under these circumstances, exploiting novel multiphase cathodes showing synergetic effect may give solution to these problems. In this review, we summarize the recent development of multiphase layered transition metal oxide cathodes of SIBs, analyze the mechanism and prospect the future potential research directions.

  • Meizhen Dai, Depeng Zhao, Xiang Wu
    Chinese Chemical Letters. 2020, 31(9): 2177-2188.

    In the past few years, the increasing energy consumption of traditional fossil fuels has posed a huge threat to human health. It is very imperious to develop the sustainable and renewable energy storage and conversion devices with low cost and environment friendly features. Hybrid supercapacitors are emerging as one of the promising energy devices with high power density, fast charge-discharge process and excellent cycle stability. However, morphology and structure of the electrode materials exert serious effect on their electrochemical performances. In this review, we summarized recent progresses in transition metal oxide based electrode materials for supercapacitors. Different synthesis routes and electrochemical performances of electrode materials and storage mechanisms of supercapacitor devices have been presented in details. The future developing trends of supercapacitor based on metal oxide electrode materials are also proposed.

  • Xiaobang Liu, Ting Yue, Kai Qi, Yubing Qiu, Bao Yu Xia, Xingpeng Guo
    Chinese Chemical Letters. 2020, 31(9): 2189-2201.

    Metal-organic frameworks (MOFs), as an emerging family of porous inorganic-organic crystal materials, exhibit widely applications in gas storage and separation, drug release, sensing, and catalysis, owing to easily adjustable pore sizes, uniformly distributed metal centers, high surface areas, and tunable functionalities. However, MOF crystal powders are usually difficult to be directly applied into specific devices because of their brittleness, insolubility and low compatibility. Therefore, to expand versatile MOF membranes with robustness and operational flexibility is urgent to satisfy practical applications. Although numerous reports have reviewed the synthesis and applications of MOF membranes, relatively few reports the electrocatalytic properties based on MOF membranes. Herein, this mini-review provides an overview of preparation of MOF membranes, including directed synthesis, secondary growth and electrochemical deposition method. Meanwhile, fabrication of ultrathin 2D MOF nanosheets those can be also defined as a kind of nanoscale MOF membranes is also mentioned. Electrocatalytic performance of oxygen reduction reaction (ORR), oxygen evolution reaction (OER), hydrogen evolution reaction (HER) and CO2 reduction reaction (CO2RR) for diverse MOF membranes/nanosheets and their derivatives are introduced.

  • Wen Shang, Huanzhou Du, Yage Wu, Jianlin Xu, Fen Ran
    Chinese Chemical Letters. 2020, 31(9): 2202-2206.

    The triblock copolymer (PAA-b-PAN-b-PAA) iSs prepared by reversible addition-fragmentation chain-transfer polymerization, and then blended with polymer (PAN) and metal hydroxide (Ni(OH)2) as a precursor for heat-treatment. A composite material of hierarchical porous nanofibers and nickel oxide nanoparticles (HPCF@NiO) is prepared by electrospinning combined with high-temperature carbonization. The effects of the ratio of PAA and PAA-b-PAN-b-PAA on the internal structure of nanofibers and their electrochemical properties as positive electrode materials are investigated. The experimental results show that when the ratio of PAA to PAA-b-PAN-b-PAA is 1.3 to 0.4, it has good pore structure and excellent electrochemical performance. At the current density of 1 A/g, the specific capacitance is 188.7 F/g and the potential window is -1 V to 0.37 V. The asymmetric supercapacitor assembled with activated carbon as the negative electrode materials has a specific capacitance of 21.2 F/g in 2 mol/L KOH and a capacitance retention of 85.7% after 12, 500 cycles at different current density.

  • Ling Jin, Xiaxia Li, Chunsen Liu, Huan Pang
    Chinese Chemical Letters. 2020, 31(9): 2207-2210.

    The construction of highly stable and regular nanoreactors is a major challenge. In this work, we use a facile template protection method to obtain ZIF-67@SiO2 (JS) and to encapsulate metal oxide nanoparticles (Co3O4) into nanoreactors (SiO2). ZIF-67 crystals provide a cobalt species; SiO2 was first used as a protective layer of ZIF-67 and then as a nanoreactor for metastable metal oxide nanoparticles. On this basis, Co3O4@SiO2 with dodecahedron morphology were synthesized by calcining JS at different temperatures, followed by a hydrothermal reaction to obtain Co3(OH)4Si2O5. Subsequently, CoSx and CoPSiO2 were fabricated through sulfuration and phosphorization. The results in this work show that nanoreactors derived from metal-organic frameworks (MOFs) with a rational structure have broad development prospects.

  • Xiu Qian, Siyu Deng, Xiang Chen, Qiang Gao, Yun-Long Hou, Aiwu Wang, Lizhuang Chen
    Chinese Chemical Letters. 2020, 31(9): 2211-2214.

    A highly stable and luminescent metal-organic framework (LMOF) with layered structure, namely, C6H4N5OZn (1) has been successfully achieved and fully characterized by single crystal X-ray diffraction, powder X-ray diffractions, fluorescence titration and thermogravimetry. This blue-light emitting compound 1 exhibit outstanding stability and can detect Fe3+ and Cu2+ in water specifically, presenting potential application in the field of fluorescent probe technology. Fluorescence titration experiments indicate that the detection of Fe3+ ions by 1 is more significant than that of Cu2+ ions in terms of Ksv value. Furthermore, guest-assisted exfoliation of layered MOF 1 is efficiently carried out through ether O—H hydrogen bond or π···π interactions between the layered host structure and intercalated guest molecules (4, 4'-oxybisbenzoic acid and triphenylamine). Tyndal scattering was observed in the suspensions of obtained MOF nanosheets. This study shows that the compound 1 with unique metal ion sensing properties can be applied as a probe material in water pollution treatment field, but also opens up the opportunity for synthesizing luminescent MONs through the "bottom-up" guest intercalation methodology.

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