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  • Yanan Gao, Jie Liu, Chenjie Lou, Hailiang Geng, Jipeng Fu, Chengyu Li, Yongjin Chen, Cong Wang, Wenda Zhang, Xiaojun Kuang, Yifan Liu, Xiang Gao, Mingxue Tang
    Chinese Chemical Letters. 2023, 34(12): 108268-.

    Anode SnO2 in lithium-ion batteries suffers from volume expansion and agglomeration. Here, the SnO2 nanoparticles are hybrided with ZrO2 particles by the support of carbon nanotube networks. The obtained SnO2/C/ZrO2 composite shows improved electrochemical performances. Investigations reveal that the carbon nanotubes shorten the transmission path of electrons and Li+ ions. Ball milling with ZrO2 promotes the formation of nanosized SnO2 to weaken the internal strain change, being beneficial to buffering volume change during electrochemical cycling afterwards. High-resolution 6, 7Li NMR investigations indicate that conversion and alloying reactions are stepwise involved for SnO2/C/ZrO2 anode. The strategy of designing SnO2/C/ZrO2 composite from the morphology-controlled metal-organic frameworks for energy storage widens the possibility to fabricate promising materials with enhanced performances.

  • Minxing Du, Yuxia Sun, Jiaojiao Zhao, Haiyan Hu, Liwei Sun, Yuehui Li
    Chinese Chemical Letters. 2023, 34(12): 108269-.

    Epoxidation is an important chemical process for the production of epoxides, key building blocks in chemical industry. Despite great efforts being made to facilitate this process, it remains a significant challenge to develop cost-effective, environmental-friendly, and selective catalysts. Herein, we reported a highly dispersed Mn supported by g-C3N4 (Mn/g-C3N4) with Mn loading up to 2.56 wt%. The Mn/g-C3N4 exhibited satisfied catalytic performance for olefin epoxidation with excellent conversion (91%), high selectivity (93%) as well as outstanding recycling stability. Further analysis revealed the importance of Mn-N structure for the generation of active oxo-containing species and subsequent oxygen atom transfer. Besides, an efficient synthesis of cyclic carbonates from styrene epoxide and CO2 has been achieved (88% conversion, 89% selectivity) based on the polar Mn-N coordinated characteristics of Mn/g-C3N4 catalyst.

  • Wenxue Zhang, Jiating Hou, Min Bai, Cheng He, Jiuran Wen
    Chinese Chemical Letters. 2023, 34(12): 108270-.

    To solve the problem of energy scarcity and widespread environmental contamination, it is necessary to design green and low-cost photocatalysts for water splitting. In this paper, a new penta-graphene/AlAs5 (PG/AlAs5) van der Waals (vdW) heterostructure is proposed and its performance for photocatalytic hydrolysis is calculated using the first-principles method. The findings suggest that the PG/AlAs5 heterostructure belong to type-Ⅱ indirect semiconductor, and the edge position and band gap width of this heterostructure satisfy the requests of redox reaction. Furthermore, the oxidation reaction (OER) on the AlAs5 side and the hydrogen evolution reaction (HER) on the PG side are thermodynamically spontaneous under different conditions. Surprisingly, the introduction of strain engineering has changed the position of the band edge and light absorption performance of PG/AlAs5 heterostructure, which is powerful for the performance of photocatalytic water splitting. The PG/AlAs5 vdW heterostructure exhibits well visible light absorption intensity without applying strain and biaxial strain of 2%. In conclusion, the findings suggest that the PG/AlAs5 vdW heterostructure is a prospecting catalyst for visible-light hydrolysis.

  • Shuang Cheng, Meng Pan, Danrong Hu, Ruxia Han, Lang Li, Zhongwu Bei, Yicong Li, Ao Sun, Zhiyong Qian
    Chinese Chemical Letters. 2023, 34(12): 108276-.

    Bacterial infection of wounds is an escalating medical problem, issuing threats to both global public health and personal health. Photothermal antibacterial technology as a novel sterilization strategy has outstanding sterilization efficiency, high safety and low risk of emergence of drug-resistant bacteria. By combining inherent antibacterial activity and light-assisted antibacterial treatment, developing novel multifunctional dressings with synergistic high-efficiency antibacterial effects and also promoting wound healing possesses attractive advantages in the field of treating bacterial wound infections in clinical care. Herein, a multifunctional hydrogel formed by in situ photo-cross linking was designed and prepared by first grafting methacrylic anhydride as a photosensitizer onto chitosan, and then introducing oxidatively synthesized polydopamine (PDA). The physicochemical characterizations of the synthesized hydrogels demonstrated their tunability certainly associated with PDA concentration, including pore size, water swelling, rheological properties and in vitro degradability. In addition, the composite hydrogels exhibited good adhesion, anti-oxidation and photothermal properties due to the existence of PDA. Within 10 min upon exposure to 808 nm near-infrared (NIR) light irradiation, this hydrogel system displayed outstanding antibacterial activity against Staphylococcus aureus with almost 100% killing efficiency, of which rapid efficient sterilization plays a significant role in wound healing. Moreover, the hydrogel is capable of cytocompatibility and has low toxicity to murine fibroblasts (L929 and NIH/3T3). In the full-thickness wound defect infection model in mice, the wound closure ratio, inflammatory response, fibroblasts, neovascularization and epithelialization were measured. Animal experiments also reveal that the hydrogel assisted with NIR laser irradiation can inhibit effectively infection at an early stage and accelerate the wound healing process. In summary, this novel multifunctional injectable hydrogel exhibits excellent swelling capacity, bio-adhesion, antioxidant property, photothermal activity, efficient antibacterial property and facilitates skin healing, which has great promising application as a medical dressing biomaterial in infected wound care fields.

  • Jinrong Huo, Kai Zhang, Haocong Wei, Ling Fu, Chenxu Zhao, Chaozheng He, Xincheng Hu
    Chinese Chemical Letters. 2023, 34(12): 108280-.

    Ammonia borane (NH3BH3, AB) is an ideal raw material of hydrogen production with higher hydrogen storage capacity. In this paper, the catalytic processes of AB dehydrogenation were described from different ways, including thermal dehydrogenation, hydrolysis, methanolysis, photocatalysis and photo-piezoelectric synergy catalysis with experimental research and theoretical calculations. Catalyst models include bulk materials, two-dimensional materials, nanocluster particles and single/diatomic structures. Among them, the proportion of H2 released is different, and the reaction conditions are also different, which are suitable for different application scenarios. Through this review, we could have a preliminary comprehensive understanding of AB dehydrogenation reaction.

  • Yaping Gong, Xiaoxian Chen, Bingqing Zhao, Jun Wang, Weixiong Zhang, Xiaoming Chen
    Chinese Chemical Letters. 2023, 34(12): 108282-.

    Two-dimensional organic-inorganic hybrid ferroelastics with high-temperature reversible phase transitions are very rare and have become one of the research hotspots in the field of ferroelastic materials. Herein, we report three new layered organic-inorganic hybrid perovskites based on halogen-substituted phenethylaminium, (3-XC6H5CH2CH2NH3)2[CdCl4] (X = F (1), Cl (2) and Br (3)). They undergo structural phase transitions at 376/371 K, 436/430 K, and 421/411 K, respectively, between the isomorphic high-temperature phases (space group I4/mmm, Z = 2) and different room-temperature phases with the reduced structural symmetries, i.e., P21/a (Z = 2) in 1, (Z = 4) in 2, and P21/a (Z = 4) in 3, respectively. These ferroelastic transitions arise from the order-disorder transition of organic cations together with the synchronous displacement of inorganic layers, accompanying with ferroelastic spontaneous strains of 0.16, 0.13 and 0.12 for 1−3, respectively. By enriching layered perovskite ferroelastics based on halogen-substituted cations, this work provides important clues for exploring new ferroic materials based on hybrid crystals.

  • Gaigai Duan, Hua Zhang, Chunmei Zhang, Shaohua Jiang, Haoqing Hou
    Chinese Chemical Letters. 2023, 34(12): 108283-.

    The trade-off between mass-loading and cycling stability is always a big challenge for iron oxide-based electrodes. Herein, α-Fe2O3 nanoparticles uniformly anchored on nitrogen-doped wood carbons with high mass-loading have been synthesized via a facile electrodeposition method accompanied by post-heating treatment. The resultant composite delivers a high specific capacitance of 603 F/g at 0.1 A/g and superior capacitance retention of 85.5% after 10,000 cycles at 10 A/g, indicating excellent long-term cycling stability. Such excellent electrochemical performance can be attributed to the synergistic effects of α-Fe2O3 nanoparticles and the conductive matrix as well as the formation of interfacial Fe-O-C bonding, which enables the composite electrode to provide plenty of accessible redox active sites, sufficient electron transport and electrolyte ions diffusion, and robust interfacial interaction. Consequently, the asymmetrical supercapacitor exhibits a high energy density of 30.3 Wh/kg at 125 W/kg, suggesting its great potential for practical applications.

  • Gongxun Yu, Fenghui Yang, Xu Han, Qiongyao Song, Jiangtao Zheng, Ying Qi, Tianming Chen, Qian Shen, Jingxia Qiu, Sheng Li
    Chinese Chemical Letters. 2023, 34(12): 108288-.

    Carbon is a promising capacitive electrode material for Zn-ion hybrid supercapacitors (ZHSCs), as it is low-cost, environmentally friendly, controllable and adjustable. By now, achieving both high energy and high power with carbon electrodes is still challenging, limited by their intrinsic properties. In this work, we have designed and presented an amorphous hollow carbon bowl material with surface chemical modifications of oxygen groups to figure out these concerns. The preparation of bowl-like structures and the storage behavior between Zn2+ and oxygen functional groups have also been discussed. With the contributions from its unique hollow structure and surface functional groups, it can significantly enhance the electrode pseudocapacitance and the entire electrochemical performance.

  • Yuan-Tao Huang, Min Xue, Yong Yang
    Chinese Chemical Letters. 2023, 34(12): 108294-.

    Tetra(amino)azacalix[4]arene skeleton was functionalized at the bridging NH sites using various aromatic aldehydes via formation of imidazobenzimidazole fused heterocycles. X-ray single crystal analysis revealed distorted 1,3-alternate conformations for the resulting macrocycles. Anthracenyl and pyrenyl modified imidazobenzimidazole fused aza-calix[4]arenes existed as dimers in the solid state, associated mainly through π-π stacking interactions between the planar polycyclic fluorophores. The tetrapyrenyl modified product was further used as a Zn2+-selective sensor, which showed naked-eye detected color change and enhanced excimer emission. The stoichiometry between the sensor and Zn2+ was determined to be 1:1 and the association constant was 1.1 × 105 L/mol. The sensing process was highly selective and showed strong anti-interference with presence of other cations. The UV-vis spectral changes in the sensing process were completely reversible by alternate addition of Zn2+ and F−, showing an efficient ''on–off-on'' result.

  • Peng Gao, Jiayun Chen, Peng Sun, Jianyou Wang, Huan Tang, Fei Xia, Liwei Gu, Huimin Zhang, Chen Wang, Yin Kwan Wong, Yinhua Zhu, Chengchao Xu, Jigang Wang
    Chinese Chemical Letters. 2023, 34(12): 108296-.

    Present research on the antimalarial mechanisms of artemisinin (ART) is mainly focused on covalent drug binding targets alkylated by free radicals, while non-covalent binding targets have rarely been reported. Here, we developed a novel photoaffinity probe of ART to globally capture and identify the antimalarial target proteins of ART through chemical proteomics. The results demonstrated that ART can bind to parasite proteins by both covalent and non-covalent modification, and these may jointly contribute to the antimalarial effects. Our work enriches the research on the antimalarial targets of ART, and provides a new perspective for further exploring the antimalarial mechanism of ART.

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