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  • Lingyuan Liu, Shuyun Zhu, Jing Sun, Meng Xia, Xian'en Zhao, Guobao Xu
    Chinese Chemical Letters. 2021, 32(2): 906-909.

    We design a ratiometric fluorescent sensing platform for bleomycin (BLM) by using proximity-dependent DNA-templated silver nanoclusters (DNA-AgNCs) probe. This ratiometric sensing system is constructed with DNA-AgNCs as single fluorophore. The proposed strategy is based on the two following facts: (1) a covert DNA can approach and transform the DNA-AgNCs with green emission (G-DNA-AgNCs) into red emission through hybridization reaction. (2) The specific cleavage of the convert DNA by BLM in the presence of Fe(II) inhibits the discoloration of G-DNA-AgNCs. Thus, benefiting from the specific recognition of BLM and unique properties of G-DNA-AgNCs, a highly-sensitive ratiometric sensor for BLM has been successfully developed. The detection limit is as low as 30 pmol/L. This label-free fluorescence probe possesses advantages of convenient synthetic process and low cost. Moreover, this ratiometric method has been applied to the detection of BLM in human serum samples, illustrating a promising tool for analysis of BLM in cancer therapy.

  • Yuantao Yan, Xiaoli Zhao, Huanglin Dou, Jingjiang Wei, Wanyu Zhao, Zhihua Sun, Xiaowei Yang
    Chinese Chemical Letters. 2021, 32(2): 910-913.

    The nano-Si/graphite nanocomposites are the promising anodes candidates for high-energy lithium-ion batteries because of their high theoretical capacities and low volume variations. However, the nano-Si has a severe tendency to separate from the graphite substrate due to the inherently weak bonding between them, thus leading to the deteriorated cycling performance and low Coulombic efficiency. Herein, we design a robust nano-Si/graphite nanocomposite structure with strong interfacial adhesion caused by the Si—Ti and Ti—C covalent bonds. The abundant Si—Ti and Ti—C bonds formed between nano-Si and graphite greatly enhance the interfacial adhesion force, resulting in the highly stabilized and integrated electrode structure during battery cycling. Consequently, the as-obtained nano-Si/graphite anodes deliver a high capacity retention of 90.0% after 420 cycles at 0.5 C with an average Coulombic efficiency of 99.5%; moreover, a high initial Coulombic efficiency of 90.2% is achieved. Significantly, this work provides a novel strategy to address the poor interfacial adhesion between nano-Si and graphite, which can be applied to other nano-Si based composites anodes.

  • Yu-Fei Lei, Xiao-Lin Wang, Bo-Wen Liu, Li Chen, Yu-Zhong Wang
    Chinese Chemical Letters. 2021, 32(2): 875-879.

    A novel kind of fully bio-based PSAs were obtained through the curing reaction between two components derived from the plant oils: carboxyl-terminated polyricinoleate (PRA) from the castor oil and epoxidized soybean oil (ESO). The gel content, glass transition temperature (Tg), rheological behavior, tensile strength, creep resistance and 180° peel strength of the PSAs were feasibly tailored by adjusting the component ratio of ESO to PRA. At low cross-linking level, the PSAs behaved like a viscous liquid and did not possess enough cohesiveness to sustain the mechanical stress during peeling. The PSAs cross-linked at or near the optimal stoichiometric conditions displayed an adhesive (interfacial) failure between the substrate and the adhesive layer, which were associated with the lowest adhesion levels. The PSAs with the dosage amount of ESO ranging from 10~20 wt% were tacky and flexible, which exhibited 180° peel strength ranging from 0.4~2.3 N/cm; and could be easily removed without any residues on the adherend. The process for the preparation of the fully bio-based PSAs was environmentally friendly without using any organic solvent or other toxic chemical, herein showing the great potential as sustainable materials.

  • Feng Su, Shuanghao Zheng, Fangyan Liu, Xiong Zhang, Fangyuan Su, Zhong-Shuai Wu
    Chinese Chemical Letters. 2021, 32(2): 914-917.

    Porous structure and heteroatom doping are two key parameters for significantly boosting the capacitive performance of graphene-based materials. Herein, we report a facile approach to prepare one-dimensional (1D) nitrogen-doped holey graphene nanoscrolls (NHGNSs) through cold quenching treatment of two-dimensional graphene oxide sheets, followed by thermal annealing in the successive atmosphere of NH3 and air. Benefiting from the synergy of the unique 1D tubular morphology, abundant nanoholes and nitrogen doping, the NHGNSs exhibit a high specific capacitance of 126 F/g at 1 A/g in ionic liquid electrolyte and excellent rate capability with 81% of the capacitance retained at 20 A/g. Furthermore, the fabricated symmetric supercapacitors based on NHGNSs achieve both high energy density of 53.5 Wh/kg at 875 W/kg and high power density of 17.5 kW/kg at 43.4 Wh/kg. The simple synthetic process and superior electrochemical performance suggest the great potential of NHGNSs for supercapacitor application.

  • Li Zhang, Dandan Wu, Gaowei Wang, Yongtai Xu, Hongxia Li, Xingbin Yan
    Chinese Chemical Letters. 2021, 32(2): 926-931.

    Zinc-ion hybrid super-capacitors are regarded as promising safe energy storage systems. However, the relatively low volumetric energy density has become the main bottlenecks in practical applications of portable electronic devices. In this work, the zinc-ion hybrid super-capacitor with high volumetric energy density and superb cycle stability had been constructed which employing the high-density three-dimensional graphene hydrogel as cathode and Zn foil used as anode in 1 mol/L ZnSO4 electrolyte. Benefiting from the abundant ion transport paths and the abundant active sites for graphene hydrogel with high density and porous structure, the zinc-ion hybrid super-capacitor exhibited an extremely high volumetric energy density of 118.42 Wh/L and a superb power density of 24.00 kW/L, as well as an excellent long cycle life (80% retention after 30,000 cycles at 10 A/g), which was superior to the volumetric energy density of the reported zinc-ion hybrid super-capacitors. This device, based on the fast ion adsorption/desorption on the capacitor-type graphene cathode and reversible Zn2+ plating/stripping on the battery-type Zn anode, which will inspire the development of zinc-ion hybrid super-capacitor in miniaturized devices.

  • Guangrui Si, Xiangjing Kong, Tao He, Wei Wu, Linhua Xie, Jianrong Li
    Chinese Chemical Letters. 2021, 32(2): 918-922.

    By taking the functional advantages of both pyrazolate and carboxylate ligands, a unique dual-functional pyrazolate-carboxylate ligand acid, 4-(3,6-di(pyrazol-4-yl)-9-carbazol-9-yl)benzoic acid (H3PCBA) was designed and synthesized. Using it, a new Co(II)-based metal-organic framework (MOF), Co3(PCBA)2(H2O)2 (BUT-75) has been constructed. It revealed a (3,6)-connected net based on the 6-connected linear trinuclear metal node, and showed good chemical stability in a wide pH range from 3 to 12 at room temperature, as well as in boiling water. Due to the presence of rich exposed Co(II) sites in pores, BUT-75 presented high selective CO2 adsorption capacity over N2 at 298 K. Simultaneously, it demonstrated fine catalytic performance for the cycloaddition of CO2 with epoxides into cyclic carbonates under ambient conditions. This work has not only enriched the MOF community through integrating diverse functionalities into one ligand but also contributed a versatile platform for CO2 fixation, thereby pushing MOF chemistry forward by stability enhancement and application expansion.

  • Bing Wu, Tianhao Xue, Yaning He
    Chinese Chemical Letters. 2021, 32(2): 932-937.

    A novel water-soluble red-emissive AIE fluorescence probe for cysteine (Cys) in situ was prepared and the performance of selectivity and sensitivity has been carefully investigated in this study. The probe was established on the electrostatic interaction of sulfonate functionalized tetraphenylethene (TPE) and polycation generated by the reaction between a polymer bearing dinitrobenzenesulfonate groups and Cys. From the experimental results, it was easy to distinguish Cys from glutathione (GSH) and homocysteine (Hcy) with a detection limit of 73 nmol/L. The assay system also possessed strong anti-interference ability against multitudinous amino acids. The Stokes shift was 142 nm and the emission ranged from 550 nm to 850 nm. In addition, double responses in fluorescence and ultraviolet-visible spectra also make the red-emissive assay ideal for sensitive detection and quantification of Cys for most purposes, especially in-situ monitoring of Cys in aqueous medium.

  • Hao Fu, Shuyu Zhou, Xi Fan, Lei Zhang, Jian Zhang
    Chinese Chemical Letters. 2021, 32(2): 923-925.

    In this work, titanium-capped cobalt clathrochelates have been applied as secondary building units (SBUs) for the construction of supramolecular rings. Two heterometallic wheel-like [Ti6Co12] complexes based on cobalt clathrochelates, [C6H15N4]2[TiCo2(μ2-Oipr)(Oipr)2(Dmg)3]6 (2, Dmg=dimethylglyoxime) and H6[TiCo2(μ2-Oipr)(Oipr)2(Dmg)3]6 (3), have been successfully synthesized and characterized. The supramolecular stacking modes of these wheels are largely dependent on the applied synthetic conditions, which further impact their gas adsorption properties.

  • Zishan Feng, Wei Zhang, Longjie Li, Bocheng Tu, Weicong Ye, Xiaofeng Tang, Hongbo Wang, Xianjin Xiao, Tongbo Wu
    Chinese Chemical Letters. 2021, 32(2): 779-782.

    We presented a low-abundance mutation detection method with lambda exonuclease and DNA three-way junction structure. The assistant strand in the DNA three-way junction structure could regulate the reaction system from the kinetics and thermodynamics aspects. The optimization of the assistant strand helps to improve the selectivity of the mutant-type DNA to the wild-type DNA about 35 times. Moreover, the cost of the optimization process could be saved by about 90%. The method was applied to the detection of a human ovarian cancer-related gene mutation BRCA1 (rs1799949, c.2082C>T). The limit of detection to the mutation abundance in the DNA three-way junction structure system (0.2%) was one order lower compared with that in the double-stranded DNA structure system (2%). The mutation abundance in different standard samples was quantitively measured, and the results were consistent with the initial abundance in the standard samples.

  • Wei Zhou, Xiangning Fang, Qinglong Qiao, Wenchao Jiang, Yue Zhang, Zhaochao Xu
    Chinese Chemical Letters. 2021, 32(2): 943-946.

    With the development of single-molecule detection and super-resolution fluorescence imaging, rhodamine dyes gain new life. Through the modification of the N-substituents and the replacement of the oxygen atom in xanthene, the wavelength and brightness can be effectively changed. However, the spectra of rhodamine, especially due to the balance between ring-closed non-fluorescent lactone and ring-opened fluorescent zwitterion/cation, are sensitive to interference from various environmental factors. In this way, the spectral data of various rhodamines reported by different research groups under different test conditions lacked comparability, sometimes even lacked accuracy. In order to meet the requirements for the accuracy and uniformity of spectral data in the research of single molecule imaging and dye structure-fluorescence relationship study, we have tested the spectra of fifteen rhodamine dyes that cover the visible and near-infrared regions under exactly the same conditions. By studying the dependence of the spectra on dye concentrations, it was confirmed that 1 μmol/L was ideal for detection less from the interference of dye molecule aggregation. We provide comprehensive and reliable spectral data of these fifteen dyes, which are expected to be used as references for future research. And the direct comparison of different rhodamine spectra would help to understand the structure-fluorescence relationship of rhodamines.

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