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  • Xiaoqing Niu, Tianbing Song, Huanming Xiong
    Chinese Chemical Letters. 2021, 32(6): 1953-1956.

    Red emissive carbon dots (CDs) powder was synthesized on a large scale from phloroglucinol and boric acid by a novel solid state reaction with yield up to 75%. This method is safe and convenient, for it needs neither high pressure reactors nor complicated post-treatment procedures. The as-prepared carbon dots powder exhibited strong red fluorescence with excitation-independent behavior. XPS measurement and PL spectra suggest that such red fluorescence arise from boron-doped structures in CDs, which increases along with the boron concentration on CDs surface but decreases when the concentration quenching effect takes place. To overcome the aggregation induced fluorescence quenching of the solid CDs powder, the conventional methods are dispersing CDs into a large amount of inert substrates. But our present work provides a new strategy to realize strong red fluorescence of CDs in solid state. As a result, such carbon dots powder works well for latent fingerprint identification on various material surfaces.

  • Qing-Wen Gui, Fan Teng, Zhou-Chao Li, Zhi-Yuan Xiong, Xue-Feng Jin, Ying-Wu Lin, Zhong Cao, Wei-Min He
    Chinese Chemical Letters. 2021, 32(6): 1907-1910.

    An efficient and eco-friendly protocol for synthesizing difluoromethylated oxindoles through a visible-light induced one-pot tandem reaction of N-arylacrylamides, difluoroacetic acid and PhI(OAc)2 was developed. This reaction proceeded in the absence of any additive, base, metal-catalyst and external photosensitizer, using cheap and easily available CHF2CO2H as the difluoromethylation reagent and bulk biomass-derived 2-MeTHF as the sole solvent. 26 Examples of N-arylacrylamide substrates were investigated, and all of them successfully underwent difluoromethylation to deliver the target products in good to excellent yields.

  • Tun Wu, Zhiyuan Jiang, Xiaobo Xue, Shi-Cheng Wang, Mingzhao Chen, Jun Wang, Haisheng Liu, Jun Yan, Yi-Tsu Chan, Pingshan Wang
    Chinese Chemical Letters. 2021, 32(6): 1911-1914.

    The reaction of a metallo-organic ligand (LA) in which two "V"-shaped bisterpyridines attaching to meta-position of "X"-shaped tetraterpyridine via < tpy-Ru2+-tpy > connectivity and Zn2+ ions gave rise to 3D supramolecular architectures: octagram (Zn8LA4). However, a position varied ligand (LB) in which two "V"-shaped bisterpyridines locating at the ortho-position of "X"-shaped tetraterpyridine afforded a different 3D hexagram (Zn6LB3). Full characterizations included NMR (1H, 13C, 2D COSY, NOESY and DOSY), ESI-MS, TWIM-MS, TEM and AFM. The resulted structures were directly determined by the position of two "V"-shaped bisterpyridines attaching to "X"-shaped tetraterpyridine.

  • Yongrui He, Xiaohong Yang, Meiling Qi, Chuanfeng Chen
    Chinese Chemical Letters. 2021, 32(6): 2043-2046.

    This work reports the investigation of a new triptycene-derived oxacalixarene (TDOC) as the stationary phase for gas chromatography (GC) with high-resolution performance for a wide range of analytes and isomers. The TDOC scaffold is composed of triptycene and 1, 8-naphthyridine moieties, inherently differing from the conventional calixarenes in structures and properties. As a result, the TDOC column exhibited outstanding column efficiency of 5679 plates/m by n-dodecane at 120 ℃. It showed advantageous performance for separations of the mixtures with various analytes and achieved high resolution of diverse isomers (skeletal, positional and cis-/trans-isomers) from apolar to polar nature. Moreover, the TDOC column exhibited high thermal stability up to 310 ℃. To date, the TDOC-based materials have not been reported in chromatography. This work demonstrates the good potential of the triptycene-derived heterocalixarenes as a new class of stationary phases for chromatographic analyses.

  • Lingzhi Chen, Xueqin Huang, Xueyi Zeng, Guiting Fang, Weijian Chen, Haibo Zhou, Xing Zhong, Huaihong Cai
    Chinese Chemical Letters. 2021, 32(6): 1967-1971.

    The sensitive and rapid detection of blood glucose is very important for monitoring and managing diabetes. Herein, a fluorescent/magnetic bimodal sensing strategy is proposed for glucose detection using a multifunction-responsive nanocomposite (MoS2 QDs-MnO2 NS). MoS2 QDs act as fluorescent probes, and MnO2 nanosheets are used as both quenchers and recognizers in this sensing platform. In the presence of glucose-mediated enzyme product (H2O2), MnO2 nanosheet is etched, thus releasing MoS2 QDs and Mn2+ ions, which causes the significantly enhancement of fluorescent and magnetic signals. Furthermore, MoS2 QDs-MnO2 NS-based fluorescent test paper is constructed for H2O2 sensing with the naked eyes. Under optimal conditions, the dual linear ranges of 20-300 μmol/L and 40-250 μmol/L toward glucose detection are obtained for the fluorescent and magnetic mode, respectively. Furthermore, this bimodal assay exhibits good reproducibility and acceptable accuracy in glucose detection of clinical samples, demonstrating great versatility and flexibility of multifunctional probes in glucose detection.

  • Mengli Lei, Xinran Zhou, Yidong Zou, Junhao Ma, Fahad A. Alharthi, Abdulaziz Alghamdi, Xuanyu Yang, Yonghui Deng
    Chinese Chemical Letters. 2021, 32(6): 1998-2004.

    The rapid development of internet and internet of things brings new opportunities for the expansion of intelligent sensors, and acetone as a major disease detection indicator (i.e., diabetes) making it become extremely important clinical indicator. Herein, uniform mesoporous ZnO spheres were successfully synthesized via novel formaldehyde-assisted metal-ligand crosslinking strategy. In order to adjust the pore structure of mesoporous ZnO, various mesoporous ZnO spheres were synthesized by changing weight percentage of Zn(NO3)2·6H2O to tannic acid (TA). Moreover, highly active heterojunction mesoporous ZnO/Co3O4 has been fabricated based on as-prepared ultra-small Co3O4 nanocrystals (ca. 3 nm) and mesoporous ZnO spheres by flexible impregnation technique. Profit from nano-size effect and synergistic effect of p-n heterojunction, mesoporous ZnO/Co3O4 exhibited excellent acetone sensing performance with high selectivity, superior sensitivity and responsiveness. Typically, 5 wt% Co3O4 embedded mesoporous ZnO sphere showed prominent acetone response (ca. 46 for 50 ppm), which was about 11.5 times higher than that in pure ZnO sensing device, and it was also endowed high cyclic stability. The nanocrystals embedded hybrid material is expected to be used as promising efficient material in the field of catalysis and gas sensing.

  • Mingsheng Xu, Mingze Sun, Sajid ur Rehman, Kangkang Ge, Xiaolong Hu, Haizhen Ding, Jichang Liu, Hong Bi
    Chinese Chemical Letters. 2021, 32(6): 2027-2032.

    The high specific capacitance along with good cycling stability are crucial for practical applications of supercapacitors, which always demands high-performance and stable electrode materials. In this work, we report a series of ternary composites of CoO-ZnO with different fractions of reduced graphene oxide (rGO) synthesized by in-situ growth on nickel foam, named as CZG-1, 2 and 3, respectively. This sort of binder-free electrodes presents excellent electrochemical properties as well as large capacitance due to their low electrical resistance and high oxygen vacancies. Particularly, the sample of CZG-2 (CoO-ZnO/rGO 20 mg) in a nanoreticular structure shows the best electrochemical performance with a maximum specific capacitance of 1951.8 F/g (216.9 mAh/g) at a current intensity of 1 A/g. The CZG-2-based hybrid supercapacitor delivers a high energy density up to 45.9 Wh/kg at a high power density of 800 W/kg, and kept the capacitance retention of 90.1% over 5000 charge-discharge cycles.

  • Xiaomeng Liu, Qishun Huang, Jun Wang, Lanling Zhao, Haoran Xu, Qing Xia, Deyuan Li, Lei Qian, Huaisheng Wang, Jintao Zhang
    Chinese Chemical Letters. 2021, 32(6): 2086-2090.

    The sluggish kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) have always restricted the development of lithium oxygen batteries (LOBs). Herein, hollow carbon spheres loaded with Pd/Pd4S heterostructure (Pd/Pd4S@HCS) were successfully prepared via the in-situ deposition to improve the electrocatalytic activities for both ORR and OER in LOBs. With the well-dispersed Pd/Pd4S nanoparticles, the hierarchical composite with large specific surface area offers favorable transport channels for ions, electron and oxygen. Especially, the Pd/Pd4S nanoparticles could exhibit excellent electrochemical performance for ORR and OER due to their intrinsic catalytic property and interfacial effect from the heterostructure. Therefore, the LOBs with Pd/Pd4S@HCS as cathode catalyst show improved specific capacities, good rate ability and stable cycling performance.

  • Mingfu Luo, Meng Wang, Huaipeng Pang, Runhao Zhang, Jing Huang, Kang Liang, Pu Chen, Peipei Sun, Biao Kong
    Chinese Chemical Letters. 2021, 32(6): 2091-2096.

    Physical adsorption is a common method to solve the contamination of methylene blue in dyeing wastewater. As a kind of adsorption material, cellulose aerogels with high porosity and surface areas have great potential application in methylene blue removal. However, the week hydrogen bonding between cellulose nanofibers making the cellulose aerogels with the poor mechanical properties and can be easily destroyed during adsorption. Hence, the preparation of cellulose aerogels with high mechanical strength is still a great challenge. Here, we report a robust super-assembly strategy to fabricate cellulose aerogels by combining cellulose nanofibers with PVA and M-K10. The resulting cellulose aerogels not only has a robust chemically cross-linked network, but also has strong H-bonds, which greatly enhance the mechanical properties. The resulting cellulose aerogels possess a low density of 19.32 mg/cm3. Furthermore, the cellulose aerogel shows 93% shape recovery under 60% strain (9.5 kPa under 60% strain) after 100 cycles, showing excellent mechanical property. The adsorption capacity of cellulose aerogel to methylene blue solution of 20 mg/L is 2.28 mg/g and the adsorption kinetics and adsorption isotherms have also been studied. Pseudo-second-order kinetic model and Freundlich isotherm model are more acceptable for indicating the adsorption process of methylene blue on the cellulose aerogel. Thus, this compressible and durable cellulose aerogel is a very prospective material for dyeing wastewater cleanup.

  • Siqi Zou, Qun Chen, Yang Liu, Yuting Pan, Gang Yao, Zhicheng Pan, Bo Lai
    Chinese Chemical Letters. 2021, 32(6): 2066-2072.

    It is well known that zero-valent iron (ZVI) could catalyze the oxidation of various oxidants to realize the rapid oxidation removal of pollutants. However, in this study, we found that the addition of different oxidants could regulate the redox function of ZVI system. In three different co-treatment systems, the effects of different oxidizers (peroxymonosulfate (PMS), persulfate (PDS), hydrogen peroxide (H2O2)) dosages on the ratios of oxidative degradation rate and reductive degradation rate of p-nitrophenol (PNP) were studied. The effect of the H+ released from oxidizers and the generated reactive oxygen species (ROS) in ZVI/PMS, ZVI/PDS, ZVI/H2O2 systems were detailed discussed. Especially, the contribution of generated ROS for reductive degradation of PNP was quantified in the ZVI/H2O2 system. Based on the results of TOC removal, UV–vis absorption spectra, and intermediates concentration curves, it was found that the degradation of PNP changed from reduction to oxidation with the increase of oxidant proportion. When the molar ratio of ZVI to oxidizer equal to 100, PNP was mainly degraded by reduction accompanied by slight oxidation. Combined with the results of SEM-EDS and XPS, it was confirmed that the enhanced degradation of PNP under the addition of oxidant was mainly related to the generated ROS, the additional H+, and the corrosion products of ZVI.

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