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  • Jingjing Wu, Tingting Hu, Guoping Zhao, Anran Li, Ruizheng Liang
    Chinese Chemical Letters. 2022, 33(10): 4437-4448.

    For more than a decade, the exfoliation of graphene and other layered materials has led to a tremendous amount of research in two-dimensional (2D) materials, among which 2D transition metal chalcogenides (TMCs) nanomaterials have attracted much attention in a wide range of applications including photoelectric devices, lithium-ion batteries, catalysis, and energy conversion and storage owing to their unique photoelectric physical properties. With such large specific surface area, strong near-infrared (NIR) absorption and abundant chemical element composition, 2D TMCs nanomaterials have become good candidates in biomedical imaging and cancer treatment. This review systematically summarizes recent progress on 2D TMCs nanomaterials, which includes their synthesis methods and applications in cancer treatment. At the end of this review, we also highlight the future prospects and challenges of 2D TMCs nanomaterials. It is expected that this work can provide the readers with a detailed overview of the synthesis of 2D TMCs and inspire more novel functional biomaterials based on 2D TMCs for cancer treatment in the future.

  • Jun Jing, Kai Qi, Guohui Dong, Mengmeng Wang, Wingkei Ho
    Chinese Chemical Letters. 2022, 33(10): 4715-4718.

    The efficiency of photocatalytic pollutant removal largely depends on the ability of the photocatalytic system to produce hydroxyl radicals (·OH). However, the capability of photocatalyst to produce ·OH is not strong at present. Advancing the capacity of photocatalytic system to produce ·OH has always been a tough problem and challenge in the field of environmental science. In this research, it was found that introducing nitric oxide (NO) into the graphitic carbon nitride (g-C3N4) photocatalytic system could memorably enhance the ability of producing ·OH group. This study provides a new idea for improving the capacity of photocatalytic ·OH production.

  • Ziyan Shen, Ning Ma, Feng Wang, Jiaming Ren, Chenxi Hou, Shuang Chao, Yuxin Pei, Zhichao Pei
    Chinese Chemical Letters. 2022, 33(10): 4563-4566.

    Nano-drug delivery systems with multiple stimulus-responsive capabilities have superior response performance and efficient drug release. Nevertheless, it is sophisticated to construct multiple stimulus-responsive systems where the two or more functional groups need to be introduced simultaneously. Xanthate, one functional group with pH and H2O2 stimulus responsiveness, has significant potential applications for building dual-responsive drug delivery system. Herein, we present a novel dual stimuli-responsive supramolecular drug delivery system by using sodium xanthate derivative (SXD) as guest molecule and quaternary ammonium capped Pillar[5]arene (QAP5) as host molecule through host-guest interaction on the basis of electrostatic interaction. The amphiphile QAP5⊃SXD could self-assemble into vesicles to efficiently load the anti-cancer drug DOX. The experimental results showed that QAP5⊃SXD nanoparticles could achieve efficient drug delivery and controlled release in the tumor microenvironment. Cytotoxicity experiments proved that DOX@QAP5⊃SXD nanoparticles could significantly improve the anticancer efficiency of free DOX on cancer cells. The present study provides an efficient strategy to develop supramolecular nanocarriers with dual-responsiveness in one functional group for controlled drug release.

  • Junwei Wang, Lei Zhao, Chen Zhu, Ben Ma, Xiaolong Xie, Jian Liu, Shiyun He, Magnus Rueping, Kun Zhao, Lihong Hu
    Chinese Chemical Letters. 2022, 33(10): 4549-4558.

    Divergent synthesis of medium-sized rings with controllable ring sizes represents a longstanding challenge in organic synthesis. Herein, we developed a transition-metal-catalyzed switchable divergent cycloaddition of para-quinone methides and vinylethylene carbonates by controlling the steric hindrance of substituent. Different from reported alkoxide-triggered annulations, this process undergoes a regiodivergent allylation of para-quinone methides followed by 1, 6-addition reaction, providing a new route to selectively synthesize seven- to ten-membered nitrogen-containing heterocycles in high yields with excellent regioselectivities. This protocol features a broad substrate scope, wide functional group tolerance as well as operational simplicity. The reaction mechanism was investigated by conducting a series of control experiments as well as DFT calculations and the origins of the regioselectivities of the cycloaddition process were rationalized.

  • Junbu Wang, Zeai Huang, Ying Wang, Jundao Wu, Zhiqiang Rao, Fang Wang, Ying Zhou
    Chinese Chemical Letters. 2022, 33(10): 4687-4690.

    The conversion of methane to syngas (H2 and CO) is an important route to produce high value-added products. Oxidize methane into syngas in the absence of gaseous oxidants is an economical route. In this work, NiO-MgO composite is successfully synthesized via an impregnation method. At 764 K, methane is directly converted to syngas on the NiO-MgO without gaseous oxidants. A synergistic effect of NiO and MgO was observed, in which NiO induced lattice oxygen of MgO mobility to oxidize methane and suppressed the formation of intermediates for side reaction. As a result, NiO-MgO exhibited enhancement of catalytic activity with the H2 production rate of 1241.0 μmol g-1 min-1, which was 3.4 times higher than that of pure MgO. This work provides a direct guidance to understand of methane oxidation via lattice oxygen under low temperature (< 773 K).

  • Huafeng Li, Mengnan Yang, Zelong Yuan, Yahao Sun, Pengtao Ma, Jingyang Niu, Jingping Wang
    Chinese Chemical Letters. 2022, 33(10): 4664-4668.

    Construction of two Ru cations and six lacunary Keggin fragments resulted in a novel Ru2W12-cluster {(RuO6)2(WO3)12(H2O)12} bridged polyoxometalate, NaH11[(RuO6)(AsW9O33)3{(W6O3)(H2O)6}]2 53H2O (NaH11·1·53H2O), which represent the largest cluster in all the Ru-containing polyoxometalates. The most interesting characteristic is that the symmetry-related Ru2W12-cluster-based hexamers contain two windmill-shaped [(RuO6)(AsW9O33)3{(W6O3)(H2O)6}] trimers or the Ru2W12 cluster was tightly wrapped by six segments of B-β-AsW9O33. The other remarkable feature is that there have one intriguing cubane structure: which is composed of the Ru(1, 2) and W(1, 28, 50, 51, 52, 53) atoms. The oxygenation reactions of anilines to azoxybenzenes was evaluated when NaH11·1·53H2O served as effective catalyst by probing various reaction. The inherent redox property of oxygen-rich polyoxometalate surfaces and high photocatalytic activity of the Ru-containing metal cluster imbedded in NaH11·1·53H2O provide sufficient driving force for the photocatalytic transformation from anilines to azoxybenzenes. The oxidation of anilines can be realized with higher selectivity to afford various azoxybenzene compounds. The durability test shows that Ru-doping catalyst displays excellent chemical stability during the photocatalytic process.

  • Jie Fu, Ching-Hua Huang, Chenyuan Dang, Qilin Wang
    Chinese Chemical Letters. 2022, 33(10): 4495-4504.

    Disinfection by-products (DBPs) in water systems have attracted increasing attention due to their toxic effects. Removal of precursors (mainly natural organic matter (NOM)) prior to the disinfection process has been recognized as the ideal strategy to control the DBP levels. Currently, biological activated carbon (BAC) process is a highly recommended and prevalent process for treatment of DBP precursors in advanced water treatment. This paper first introduces the fundamental knowledge of BAC process, including the history, basic principles, typical process flow, and basic operational parameters. Then, the selection of BAC process for treatment of DBP precursors is explained in detail based on the comparative analysis of dominant water treatment technologies from the aspects of mechanisms for NOM removal as well as the treatability of different groups of DBP precursors. Next, a thorough overview is presented to summarize the recent developments and breakthroughs in the removal of DBP precursors using BAC process, and the contents involved include effect of pre-BAC ozonation, removal performance of various DBP precursors, toxicity risk reduction, fractional analysis of NOM, effect of empty bed contact time (EBCT) and engineered biofiltration. Finally, some recommendations are made to strengthen current research and address the knowledge gaps, including the issues of microbial mechanisms, toxicity evaluation, degradation kinetics and microbial products.

  • Demei Zhang, Shiyu Yang, Xiaoyu Fang, Huifeng Li, Xuebo Chen, Dongpeng Yan
    Chinese Chemical Letters. 2022, 33(10): 4669-4674.

    The existing industrial ammonia synthesis usually adopts the Haber-Bosch process, which requires harsh conditions of high temperature and high pressure, and consumes high energy. Under this circumstance, photoelectrochemical (PEC) catalysis is regarded as a promising method for N2 reduction reaction (NRR), but bears problems of low efficiency and yield. Thus, exploring active catalysts remains highly desirable. In this work, BiVO4@MXene hybrids have been facilely synthesized by a hydrothermal route. The heterojunctions by the in situ growth of BiVO4 onto two-dimensional (2D) MXene greatly increase the NRR efficiency: under photoelectric conditions, the optimized NH3 yield is 27.25 μg h -1 cm-2, and the Faraday efficiency achieves 17.54% at -0.8 V relative to the reversible hydrogen electrode (RHE), which are higher than most state-of-the-art NRR (photo) electrocatalysts. The mechanism speculation shows the enhanced light absorption range and the heterojunction formation largely promote the separation and the transfer efficiency of photogenerated carriers, thereby improving the PEC catalytic ability. Therefore, this work provides a hybrid route to combine the advantages of photo and electric catalysis for effective artificial nitrogen fixation.

  • Yunxia Wang, Chuangxin Zhang, Hui Zhang, Liheng Feng, Libing Liu
    Chinese Chemical Letters. 2022, 33(10): 4605-4609.

    It is of great significance to develop effective antibacterial agents and methods to combat drug resistant bacterial infections due to its increasing threaten to human health and the ineffectiveness of antibiotics. Herein, a multifunctional hybrid nano-assembly (M1-Fe NPs) based on conjugated oligomer and ferrous ion was engineered with favorable bactericidal activity for synergetic antibacterial therapy. The chelation of ferrous ion not only enhances the photothermal conversion efficiency of M1 but also endows the nano-assembly with catalytic capability of transferring H2O2 into stronger oxidant hydroxyl radicals (OH). Meanwhile, the generated heat can further promote the Fenton reaction activity. By generating cytotoxic heat and oxidative OH, M1-Fe NPs can effectively kill Staphylococcus aureus in vitro and in vivo with the aid of low dosage of H2O2. The work provides a new multifunctional platform for combinational drug resistant antibacterial therapy and even antitumor therapy.

  • Wei Wu, Yi You, Zhiqiang Weng
    Chinese Chemical Letters. 2022, 33(10): 4517-4530.

    Fluoroalkyl-containing organic compounds have exhibited wide applications in the field of pharmaceuticals, agrochemicals and materials science due to their outstanding properties such as biological activity, metabolic stability, lipophilicity, excellent chemical and thermal stability. Therefore, various synthetic strategies have been developed for the construction of fluoroalkyl-containing compounds, using highly active fluorinating reagents and fluorinated building blocks. Recently, the use of easily available and inexpensive trifluoroacetic anhydride (TFAA) and its anhydride analogues has attracted great attention to access numerous fluoroalkyl-containing compounds through cyclization and coupling reactions. In this review, we summarized the recent advances in the synthesis of fluoroalkylated compounds using fluoroalkyl anhydrides as reagents. This review aims to provide a reference for researchers on how to develop new synthetic straregies of fluorine-containing organic compounds and achieve kilograms or even tons preparation of fluorine-containing organic compounds using fluoroalkyl anhydrides.

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