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  • Jianan Su, Linzhou Zhuang, Shusheng Zhang, Qingju Liu, Longzhou Zhang, Guangzhi Hu
    Chinese Chemical Letters. 2021, 32(10): 2947-2962.

    Single atom catalyst (SAC) refers to a novel catalyst with the active metal atoms individually anchored on the support. Single atom catalysts present the unique appeal due to the high atomic availability and specific activity, as well as the high pathway selectivity. Herein, we summarized the classification, preparation, characterization, and application of single atom catalysts. Finally, the current bottlenecks and the outlooks of the SAC research are discussed.

  • Zi-Ying Li, Zhao-Quan Yao, Rui Feng, Ming-Hua Sun, Xiao-Tian Shan, Zi-Hao Su, Wei Li, Xian-He Bu
    Chinese Chemical Letters. 2021, 32(10): 3095-3098.

    A highly stable fluorescent terbium MOF (Tb4(paip)6·1.2H2O, paip=5-(1H-pyrazole-4-yl)isophthalate) showing a sharp green emission (545 nm) and a quantum yield of 21.0% was successfully synthesized. This compound is shown to be a recyclable sensor for detecting picric acid in aqueous solution with both high sensitivity and selectivity, attributed to the electron transfer quenching mechanism.

  • Xiangling Ren, Xinyuan Huang, Qiong Wu, Longfei Tan, Changhui Fu, Yi Chen, Xianwei Meng
    Chinese Chemical Letters. 2021, 32(10): 3087-3089.

    Tumor cells usually show abnormally high glycolysis rate to maintain the dynamic balance of energy. The growth of tumor cells can be affected by inhibiting the activity of pyruvate kinase (especially M2-type isozyme, PKM2), the rate limiting enzyme of glycolysis. This is helpful to the treatment of tumor. Herein, metal organic frameworks (MOFs) were found to inhibit the activity of PKM2. Nanoscale ZIF-8 was synthesized by standing and ultrasonic method, respectively. The ZIF-8 has the performance of inhibiting PKM2. Further research showed that the inhibition ability was attributed to zinc ion in ZIF-8. Interestingly, the IC50 of ZIF-8 on PKM2 was one percent of that of zinc ion. This novel enzyme inhibitor is expected to be used in cancer therapy.

  • Fenfen Zhou, Yanli Zhou, Jianwei Zhang, Hui Dong, Lantao Liu, Yintang Zhang, Maotian Xu
    Chinese Chemical Letters. 2021, 32(10): 3155-3158.

    Accurate detection of hydrogen sulfide (H2S) is of great significance for environmental monitoring and protection. We propose a colorimetric method for the detection of H2S by the use of mixed-node Cu-Fe metal organic frameworks (Cu-Fe MOFs) as highly efficient mimic enzymes for target-induced deactivation. The Cu-Fe MOFs were synthesized by a simple solvothermal method and could catalyze the H2O2 mediated oxidation of 3, 3′, 5, 5′-tetramethylbenzidine (TMB) to oxTMB with a blue color. The presence of dissolved H2S would deactivate the mimic enzymes, and then the blue color disappeared. The mechanism of the sensor was discussed by steady-state kinetic analysis. The designed assay was highly sensitive for H2S detection with a linear range of 0−80 μmol/L and a detection limit of 1.6 μmol/L. Moreover, some potential substances in the water samples had no interference. This method with the advantages of low cost, high sensitivity, selectivity, and visual readout with the naked eye was successfully applied to the determination of H2S in industrial wastewater samples.

  • Ronghua Jin, Zhongning Liu, Tao Liu, Pingyun Yuan, Yongkang Bai, Xin Chen
    Chinese Chemical Letters. 2021, 32(10): 3076-3082.

    Chemotherapy is one of the most conventional modalities for cancer therapy. However, the high multidrug resistance of tumor cells still limited the clinical application of current chemotherapy. Considering the ability of nitric oxide (NO) to modulate potent P-glycoprotein to inhibit multi-drug resistance, a synergistic methodology combining chemotherapy and sustained NO generation is an ideal way to further promote the chemotherapy. Herein, a multi-functional micelle with tumor-selective chemotherapy driven by redox-triggered doxorubicin (DOX) release and drug resistance inhibition based on intracellular NO generation was fabricated for effective tumor treatment. The micelle consists of DOX as core, arginine/glucose oxidase (Arg/GOx) as shell and redox-responsive disulfide bond as a linker, which is denoted as micelle-DOX-Arg-GOx. The Arg serves as the biological precursor of nitric oxide for inhibition of multi-drug resistance to promote chemotherapy and GOx catalyzes glucose to produce hydrogen peroxide (H2O2) for increasing the generation of NO. Moreover, the glucose supply could be simultaneously blocked by the catalytic process, which further enhanced therapeutic efficiency. This micelle requests a tumor-specific microenvironment (a considerable amount of GSH) to perform synergistic therapeutics including chemotherapy, starvation therapy (catalytic medicine), and gas therapy for tumor treatment, which resulted in significant cytotoxicity to tumor tissue.

  • Xue-Fei Tan, Shi-Shu Zhu, Ru-Peng Wang, Yi-Di Chen, Pau-Loke Show, Feng-Fa Zhang, Shih-Hsin Ho
    Chinese Chemical Letters. 2021, 32(10): 2939-2946.

    Biochar (BC) are widely used as highly efficient adsorbents to alleviate aromatics-based contaminants due to their ease of preparation, wide availability, and high sustainability. The surface properties of BCs usually vary greatly due to their complex chemical constituents and different preparation processes and are reflected in the values of parameters such as the specific surface area (SSA), pore volume/size, and surface functional groups (SFGs). The effects of SSA and pore volume/size on the adsorption of aromatics have been widely reported. However, the corresponding mechanisms of BC SFGs towards aromatics adsorption remains unclear as the compositions of the SFGs are usually complex and hard to determine. To address in this gap in the literature, this review introduces a new perspective on the adsorption mechanisms of aromatics. Through collecting previously-reported results, the parameters logP (logarithm of the Kow), polar surface area, and the positive/negative charges were carefully calculated using ChemDraw 3D, which allowed the hydrophobicity/hydrophilicity properties, electron donor-acceptor interactions, H-bonding, and electrostatic interactions between SFGs and aromatics-based contaminates to be inferred intuitively. These predictions were consistent with the reported results and showed that tailor-made BCs can be designed according to the molecular weights, chemical structures, and polarities of the target aromatics. Overall, this review provides new insight into predicting the physicochemical properties of BCs through revealing the relationship between SFGs and adsorbates, which may provide useful guidance for the preparing of highly-efficient, functional BCs for the adsorption of aromatics.

  • Xixi Pang, Yingtao Zhao, Xiangxiang Gao, Guoqi Wang, Hao Sun, Jun Yin, Jian Zhu
    Chinese Chemical Letters. 2021, 32(10): 3099-3104.

    Recently discovered bismuth oxychalcogenide (Bi2O2Se) has aroused great interest due to its ultrahigh carrier mobility, tunable band gap and good environmental stability, making it a promising candidate for high-performance electronics and optoelectronics. Their synthesis by colloidal approaches represents a cost-effective alternative to well-established chemical vapor deposition methods, and the resulting electronic-grade inks are important for large-area printed or wearable electronics. However, it is still challenging to control the colloidal growth of Bi2O2Se nanosheets in solution in addition to their assembly into high-performance thin films. Here, we report a two-step colloidal synthesis of Bi2O2Se nanosheets by separating the seeding and growth steps, thereby achieving controllable production of nanosheets with a lateral size of 1.4 μm and a thickness of 10 nm at optimized reaction conditions. These Bi2O2Se nanosheets are electrostatically assembled into large-area thin films, from which a photodetector is fabricated with a responsivity of 6.1 A/W and a short response time of 368 μs under the 520-nm laser illumination. The device exhibits fast response to modulations as high as 100 kHz, along with a −3 dB bandwidth of 1 kHz. This work provides an important understanding of the controlled colloidal synthesis of Bi2O2Se nanosheets, and demonstrates their potential applications in fast photodetectors.

  • Yiwei Zhao, Haifeng Yuan, Xiaofei Zhang, Guobin Xue, Jiebin Tang, Yuke Chen, Xiaoli Zhang, Weijia Zhou, Hong Liu
    Chinese Chemical Letters. 2021, 32(10): 3090-3094.

    The Co@NCNTs/Si pillars with channels is assemble to a suitable pure water gathering device, which is applied in seawater desalination and sewage purification to produce pure water by utilizing solar energy. High-efficiency utilization of solar energy to generate water vapor is popular, recyclable, and environmentally friendly for seawater desalination and sewage purification, helping to alleviate the global water shortage crisis. Here, we report an efficient and simple method to prepare a three-dimensional (3D) evaporator for steam generation by harnessing the power of the sun. This evaporation is composed of one-dimensional (1D) cobalt embedded and nitrogen doped carbon nanotubes (Co@NCNTs) and 3D silicon pillars array structure (Si pillars). The Co@NCNTs/Si pillars shows a wide light absorption range provided by carbon nanotubes and a long light absorption path because of the silicon pillars. The surface temperature of the sample rises rapidly in 1.5 min and exceed 80 ℃ under solar illumination of one sun. The water evaporation can be high as 1.21 kg m−2 h−1 under one sun irradiation (1 kW/m2) with the energy efficiency up to 82.4%. This scalable Co@NCNTs/Si pillars can prepare pure water from seawater and sewage, where the removal rate of ions in seawater and pollutants in sewage is similar to 100%. Based on our research, this multistage three-dimensional structure is a simple and efficient novel photothermal material for extensive seawater desalination and sewage purification.

  • Jie Liu, Miao Ben, Andeng Liu, Jianwen Liu, Shiquan Wang, Jiujun Zhang
    Chinese Chemical Letters. 2021, 32(9): 2914-2918.

    The silicon-based materials are promising candidates for lithium-ion batteries owing to their high energy density. However, achieving long lifespan under realistic conditions remains a challenge because of the volume expansion and low conductivity. In this work, the highly elastic cobweb-like composite materials consisted by SiO and nanofibers are designed and fabricated for high-efficient lithium storage by ball-milling & ; electrostatic spinning method. The reconstructed heterostructure and highly elastic nanofibers can simultaneously increase the conductivity and inhibit the "expansion effect" of silicon-based materials. The constructed electrode of n-SiO/CNF delivers an initial capacity of 1700 mAh/g, and maintains the capacities over 1000 mAh/g after 100 cycles at the current density of 500 mA/g. Meanwhile, this electrode can give an initial coulombic efficiency over 85% and maintains at 98% in the following charge/discharge processes. Furthermore, it exhibits efficient long-term electrochemical performance, maintaining the capacity at about 1000 mAh/g at a high current density of 1000 mA/g after 1000 cycles. This work could provide a promising strategy for enhancing the performance of silicon-based composite materials for practical application in lithium-ion batteries.

  • Wei Huang, Ming-Liang Han, Yu-Wen Liu, Hui Xu, Hui-Xiong Dai
    Chinese Chemical Letters. 2021, 32(9): 2765-2768.

    We report herein a palladium-catalyzed diarylative dearomatization of indole by employing thioester and arylboronic acid as the aryl electrophiles. The reaction involved a decarbonylation/migratory insertion/terminal Suzuki coupling procedure. Substrates bearing various functional groups are well tolerated in the reaction, affording the diarylated indoline skeletons in moderate to good yields.

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