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  • Yapiao Li, Qiang Zhao
    Chinese Chemical Letters. 2020, 31(7): 1982-1985.

    Fluorescence anisotropy (FA) assay in homogenous solution is simple, sensitive and reproducible. Here, we reported an aptamer structure switch FA assay for detection of aflatoxin B1 (AFB1), one of the most toxic mycotoxins, by using tetramethylrhodamine (TMR)-labeled aptamer probe and its complementary DNA (cDNA) with tandem G bases extension, to meet the demand in sensitive and selective detection of AFB1. The hybridization of aptamer and cDNA drew TMR close to the repeated guanine (G) bases, and a high FA value was induced due to TMR-G interaction and restricted local rotation of TMR. In the presence of AFB1, aptamer bound to AFB1 instead of the cDNA due to competition. Thus, the TMR-G interaction was eliminated, and FA value of TMR decreased. This assay enabled the detection of AFB1 with detection limit of 125 pmol/L and dynamic range from 125 pmol/L to 31.2 nmol/L

  • Feng Wang, Lian Chen, Huiling Li, Gaigai Duan, Shuijian He, Lin Zhang, Guoying Zhang, Zhengping Zhou, Shaohua Jiang
    Chinese Chemical Letters. 2020, 31(7): 1986-1990.

    Biomass-derived porous carbon with developed pore structure is critical to achieving high performance electrode materials. In this work, we report a grape-based honeycomb-like porous carbon (GHPC) prepared by KOH activation and carbonization, followed by N-doping (NGHPC). The obtained NGHPC exhibits a unique honeycomb-like structure with hierarchically interconnected micro/mesopores, and high specific surface area of 1268 m2/g. As a supercapacitor electrode, the NGPHC electrode exhibits a remarkable specific capacitance of 275 F/g at 0.5 A/g in a three-electrode cell. Moreover, the NGHPC//NGHPC symmetric supercapacitor displays a high energy density of 12.6 Wh/kg, and excellent cycling stability of approximately 95.2% capacitance retention after 5000 cycles at 5 A/g. The excellent electrochemical performance of NGHPC is ascribed to its high specific surface area, honeycomb-like structure and high-content of pyrodinic-N (36.29%). It is believed that grape-based carbon materials show great potential as advanced electrode materials for supercapacitors.

  • Zhi-Peng Yu, Xue Li, Chengliang He, Di Wang, Ran Qin, Guanqing Zhou, Zhi-Xi Liu, Thomas Rieks Andersen, Haiming Zhu, Hongzheng Chen, Chang-Zhi Li
    Chinese Chemical Letters. 2020, 31(7): 1991-1996.

    The recent evolution of active components yielded brilliant progresses for organic solar cells (OSCs), yet the mechanism is needed to be clearly understood. In this work, two electron acceptors, a linear SN6-2Br and a V-shaped BTP-2Br, are developed with nitrogen atoms introduced to replace the traditional sp3-hybridized carbon in the fused ring. BTP-2Br possesses an electron-deficient central core, which exhibits slightly blue-shifted absorption as well as deepened HOMO-level compared with SN6-2Br. The corresponding photovoltaic performance from V-shaped BTP-2Br based devices exhibit superior performance especially in short-circuit current (Jsc), despite an enhanced absorption and charge carrier mobilities for SN6-2Br. The primary reason for the higher Jsc from BTP-2Br is faster exciton diffusion and dissociation in blends, than those of SN6-2Br. As a result, PBDB-TF:BTP-2Br based devices achieve a power conversion efficiency (PCE) of 13.84% with an voltage-loss of only 0.46 V, which is one of the lowest values ever reported. Moreover, we fabricated semitransparent OSCs that exhibit an excellent PCE of 9.62% with average visible transparency of 20.1%.

  • Cuicui Zhu, Yiping Wang, Ling Shuai, Yizhao Tang, Ming Qiu, Jian Xie, Jia Liu, Wen Wen, Hengquan Chen, Suifei Nan, Mei Dou, Qinggang He
    Chinese Chemical Letters. 2020, 31(7): 1997-2002.

    Nonaqueous Li-O2 batteries attract attention for their theoretical specific energy density. However, due to the difficulty of decomposition of Li2O2, Li-O2 batteries have high charge overpotential and poor cycling life. So all kinds of catalysts have been studied on the cathode. Compared to heterogeneous solid catalysts, soluble catalysts achieve faster and more effective transport of electrons by reversible redox pairs. Here, we first report ruthenocene (Ruc) as a mobile redox mediator in a Li-O2 battery. 0.01 mol/L Ruc in the electrolyte effectively reduces the charging voltage by 610 mV. Additionally, Ruc greatly increases the cycling life by four-fold (up to 83 cycles) with a simple ketjen black (KB) cathode. The results of SEM, XPS and XRD confirm that less discharge product residue accumulated after recharge. To verify the reaction mechanisms of the mediator, free energy profiles of the possible reaction pathways based on DFT are provided.

  • Bingqian Xu, Wan Jiang, Lianjun Wang, Binota Thokchom, Pengpeng Qiu, Wei Luo
    Chinese Chemical Letters. 2020, 31(7): 2003-2006.

    Sulfate radical anion (SO4·-) based Fenton-like reaction have recently received a large quantity of attention owing to their strong oxidative capacity and high selectivity toward organic pollutants. However, the development of a high-efficient catalyst for activation of peroxymonosulfate (PMS) with a fast separation is still challengeable. Herein, magnetic mesoporous silica composites with a yolk-shell structure (Fe@void@mSiO2) have been prepared via a successive coating strategy, followed by a hightemperature in-situ treatment and demonstrated as a high-efficient and fast magnetic separable catalyst for the activation of PMS. The resultant material possesses a well-defined yolk-shell structure with high specific surface area (~495.0 m2/g), uniform pore size (~6.9 nm) and super large magnetic susceptibility (~105 emu/g). Owing to the unique properties, the material possesses an excellent degradation activity for tetracyclines (TC), which is much higher than the commercialized Zero Valent Iron (ZVI) nanoparticles. Additionally, the catalyst is able to work over a broad pH range and be quickly recycled by using an external magnetic field. This research provides a promising strategy for the synthesis and design of multifunctional catalyst for the Fenton-like process.

  • Guangmeng Qu, Xixi Zhang, Guotao Xiang, Yunrui Wei, Jiangmei Yin, Zonghua Wang, Xiaoli Zhang, Xijin Xu
    Chinese Chemical Letters. 2020, 31(7): 2007-2012.

    Nano-polyhedral NiSe2/CoSe2 (Ni-Co-Se) with hollow architectures are synthesized by selenizing the precursors of Ni-Co bimetallic hydroxides that are directly derived from ZIF-67. The as-fabricated Ni-Co-Se electrodes exhibit high specific capacitance of 1668 F/g at 1 A/g accompanying with outstanding rate capability (about 82.8% retention of the initial capacity at 20 A/g). The corresponding Ni-Co-Se//AC all-solid-state hybrid supercapacitors are assembled by directly using the Ni-Co-Se on carbon fabric as the positive electrode, which deliver high energy density and power density (38.5 Wh/kg at 802.1 W/kg, 32.0 Wh/kg at 8008.8 W/kg), excellent cyclic stability (82.3% retention after 5000 cycle) and robust mechanical flexibility (no obvious attenuation at bending to different angles). This work will provide a new and smart route for constructing transition metal selenides for supercapacitor devices.

  • Bo Wang, Pitsiri Sukkaew, Guichen Song, Andreas Rosenkranz, Yunxiang Lu, Kazhihito Nishimura, Jia Wang, Jilei Lyu, Yang Cao, Jian Yi, Lars Ojamäe, He Li, Nan Jiang
    Chinese Chemical Letters. 2020, 31(7): 2013-2018.

    4H-silicon carbides deposited by diamond films have wide applications in many fields such as semiconductor heterojunction, heat sink and mechanical sealing. Nucleation plays a critical role in the deposition of the diamond film on 4H-silicon carbides. Nevertheless, as a typical polar material, the fundamental mechanism of diamond nucleation on different faces of 4H-silicon carbides has not been fully understood yet. In this contribution, nucleation of diamond was performed on the carbon- and silicon-faces of 4H-silicon carbides in a direct current chemical vapor deposition device. The nucleation density on the carbon-face is higher by 2-3 orders of magnitude compared to the silicon-face. Transmission electron microscopy verifies that there are high density diamond nuclei on the interface between the carbon-face and the diamond film, which is different from columnar diamond growth structure on the silicon-face. Transition state theory calculation reveals that the unprecedented distinction of the nucleation density between the carbon-face and the silicon-face is attributed to different desorption rates of the absorbed hydrocarbon radicals. In addition, kinetic model simulations demonstrate that it is more difficult to form CH2(s)-CH2(s) dimers on silicon-faces than carbon-faces, resulting in much lower nucleation densities on silicon-faces.

  • Jiapeng Zhang, Fanzhen Lin, Lijing Yang, Zhaoyi He, Xiaoshan Huang, Dingwei Zhang, Hua Dong
    Chinese Chemical Letters. 2020, 31(7): 2019-2022.

    In this work, a series of chitin-supported Ru catalysts, composed of ultrasmall Ru nanoparticles supported on the chitin nanofibers, with different Ru content from 0.07 wt% to 0.93 wt%, are fabricated. Results from catalyzed NaBH4 hydrolysis experiments indicate that the catalytic activity of the fabricated chitin-supported Ru catalysts increases gradually with the decreasing of Ru content. The rate of hydrogen generation from NaBH4 hydrolysis catalyzed by the catalyst with 0.07 wt% Ru content is as high as 55.29 L min-1 at 30 ℃, and this reaction exhibits activation energy of 39.16 kJ/mol. The augment of NaBH4 dosage in the experiments does not weaken the catalytic activity. In addition, the fabricated chitin-supported Ru catalysts show excellent durability in NaBH4 hydrolysis, with only 9.2% activity loss after used for 20 cycles. With excellent catalytic activity and durability, the as-obtained Ru catalysts provide a promising choice for promoting hydrogen production from NaBH4 hydrolysis.

  • Kongzhao Su, Shunfu Du, Wenjing Wang, Daqiang Yuan
    Chinese Chemical Letters. 2020, 31(7): 2023-2026.

    The controlled self-assembly of discrete metal-organic nanocapsules (MONCs), and metal-organic frameworks (MOFs) based on the MONCs are achieved. Specifically, the solvothermal reaction of nickel nitrate hexahydrate and C-methylpyrogallol[4]arene in mixed DMF/MeOH solution leads to the unexpected form of discrete nickel-seamed hexameric pyrogallol[4]arene MONCs, and MONC-based three-dimensional (3D) MOF. Notably, the latter MOF is constructed from the aforementioned nickelseamed MONC building blocks and formate linkers in-situ generated from the hydrolysis of DMF solvent. Interestingly, introducing pyridine and formic acid in the reaction conditions leads to the controlled assemblies of the discrete MONC and MONC-based 3D MOF structures. Moreover, the variabletemperature magnetic susceptibilities of both the abovementioned compounds have been investigated, indicating typical antiferromagnetic interactions between the metal centers.

  • Zhaoqing Shi, Qianqian Li, Lin Mei
    Chinese Chemical Letters. 2020, 31(6): 1345-1356.

    Cancer is one of the diseases that have the highest mortality, which threatens the human health. Chemotherapy functions as the most widely used strategy in clinic to treat cancer, still exists urgent problems, like lacking selectivity and causing severe side effects. According to detailed researches on the metabolism, functions and histology of cancer tissues, many different features of cancer are uncovered, like lower pH in microenvironment, abnormal redox level in intracellular compartments and elevated expression level of several enzymes and receptors. Recently, the development of smart nanoparticles that response to tumor specific microenvironment has lighted up hope for selective cancer therapy. Herein, this review mainly focuses on pH-sensitive nanoscale materials for anti-cancer drug delivery. We summarized the formation progress of acidic tumor microenvironment, the mechanism of pH-responsive drug delivery system and nanomaterials that responsive to acidic pH in tumor microenvironment.

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