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  • Chang Xu, Zhize Liu, Xi Chen, Yang Gao, Wenjun Wang, Xijing Zhuang, Hao Zhang, Xufeng Dong
    Chinese Chemical Letters. 2024, 35(2): 109197-.

    Bone damage caused by trauma and tumors is a serious problem for human health, therefore, three-dimensional (3D) scaffolding materials that stimulate and promote the regeneration of broken bone tissues have become the focus of current research in the field of bone damage repair. To this regard, a preferential combination of materials and preparation techniques is considered crucial for the preparation of advanced bone tissue engineering scaffolds to better facilitate the regeneration of broken bone. In this review, current research advances and challenges in bone tissue engineering scaffolds are discussed and analyzed in detail. First, we elucidated the structure and self-healing mechanism of bone tissue. Subsequently, the main applications of different materials, including inorganic and organic materials, in bone tissue engineering scaffolds are summarized. Moreover, we overview the latest research progress of the mainstream preparation strategies of bone tissue engineering scaffolds, and provide an in-depth analysis of the different advantages of each method. Finally, promising future directions and challenges of bone tissue engineering scaffolds are systematically discussed.

  • Hui Cheng, Yueming Liu, Zhongling Cheng, Xianying Wang, Na Huang, Haijiao Zhang
    Chinese Chemical Letters. 2024, 35(2): 108923-.

    Si-based materials have shown great potential as lithium-ion batteries (LIBs) anodes due to their natural reserves and high theoretical capacity. However, the large volume changes during cycles and poor conductivity of Si lead to rapid capacity decay and poor cycling stability, ultimately limiting their commercial applications. Herein, we have skillfully utilized the microporous MCM-22 zeolite as the unique silicon source to produce porous Si (pSi) sheets by a simple magnesiothermic reduction, followed by a carbon coating and further Ti3C2Tx MXene assembly, obtaining the ternary pSi@NC@TNSs composite. In the design, porous Si sheets provide more active sites and shorten Li-ion transport paths for electrochemical reactions. The N-doped carbon (NC) layer serves as a bonding layer to couple pSi and Ti3C2Tx. The conductive network formed by 2D Ti3C2Tx and medium NC layer effectively enhances the overall charge transport of the electrode material, and helps to stabilize the electrode structure. Therefore, the as-made pSi@NC@TNSs anode delivers an improved lithium storage performance, exhibiting a high reversible capacity of 925 mAh/g at 0.5 A/g after 100 cycles. This present strategy provides an effective way towards high-performance Si-based anodes for LIBs.

  • Yufen Lv, Hongyu Ding, Jinmao You, Wei Wei, Dong Yi
    Chinese Chemical Letters. 2024, 35(2): 109107-.

    An additive-free and environmentally friendly strategy has been realized for the construction of S-substituted isothioureas through visible-light-induced multicomponent reaction starting from α-diazoesters, aryl isothiocyanates, amines and cyclic ethers. This methodology features simple operation, mild reaction conditions, favorable functional group tolerance, easily available starting materials and high efficiency.

  • Jin Wang, Qingqing Zhang, Yanchen Li, Xiaoyan Pan, Yuanyuan Shan, Jie Zhang
    Chinese Chemical Letters. 2024, 35(2): 108746-.

    Remodeling tumor microenvironment (TME) is a very promising and effective strategy to enhance the effects of chemotherapy, photodynamic therapy, and immunotherapy. Normalization of tumor vasculature as well as depletion of glutathione (GSH) can improve the TME. Here, we developed a novel therapeutic nanoparticle functional enzyme ultra QDAU5 nanoparticles (FEUQ Nps) based on a fluorescence-on and releasable strategy by combining a vascular normalization inducer, a GSH depleting agent, and an activated fluorophore. In which the cleavage of disulfide bonds releases active molecules that induce vascular normalization and improve the hypoxic microenvironment. In addition, it may deplete GSH in cancer cells, thus inducing the production of reactive oxygen species (ROS) and lipid peroxide (LPO) and promoting iron toxicity. It may also lead to endoplasmic stress and release of calmodulin, which activates the immune system. Meanwhile, quenched fluorophores are turned on in the presence of galactosidase (GLU) for tumor-specific labeling. In summary, we developed novel therapeutic agent nanoparticles with the function of vascular normalization inducers to achieve specific labeling of hepatocellular carcinoma while exerting efficient antitumor effects in vivo.

  • Hanwen Jian, Kaiming Deng, Tongyu Wang, Chengxi Huang, Fang Wu, Hailing Huo, Bo Ouyang, Xuan Liu, Jingjing Ma, Erjun Kan, Ang Li
    Chinese Chemical Letters. 2024, 35(2): 108651-.

    The efficiency of photocatalytic CO2 reduction reaction (PCRR) is restricted by the low solubility and mobility of CO2 in water, poor CO2 adsorption capacity of catalyst, and competition with hydrogen evolution reaction (HER). Recently, hydrophobic modification of the catalyst surface has been proposed as a potential solution to induce the formation of triple-phase contact points (TPCPs) of CO2 (gas phase), H2O (liquid phase), and catalysts (solid phase) near the surface of the catalyst, enabling direct delivery of highly concentrated CO2 molecules to the active reaction sites, resulting in higher CO2 and lower H+ surface concentrations. The TPCPs thus act as the ideal reaction points with enhanced PCRR and suppressed HER. However, the initial synthesis of triple-phase photocatalysts tends to possess a lower bulk density of TPCPs due to the simple structure leading to limited active points and CO2 adsorption sites. Here, based on constructing a hydrophobic hierarchical porous TiO2 (o-HPT) with interconnected macropores and mesopores structure, we have significantly increased the density of TPCPs in a unit volume of the photocatalyst. Compared with hydrophobic macroporous TiO2 (o-MacPT) or mesoporous TiO2 (o-MesPT), the o-HPT with increased TPCP density leads to enhanced photoactivity, enabling a high methanol production rate with 1111.5 µmol g−1 h−1 from PCRR. These results emphasize the significance of high-density TPCPs design and propose a potential path for developing efficient PCRR systems.

  • Hongjie Xu, Yujie Su, Chenggong Zheng, Yuchen Wang, Yuping Tong, Zhongzheng Yang, Junhua Hu
    Chinese Chemical Letters. 2024, 35(2): 109173-.

    In recent years, due to the increasing demand for portable electronic devices, rechargeable solid-state battery technology has developed rapidly. Lithium-ion batteries are the systems of choice, offering high energy density, flexible and lightweight design, and longer lifespan than comparable battery technologies. Therefore, a better understanding of the relationship between electrochemical mechanism and structural properties from theory and experiment will enable us to accelerate the development of high-performance and security batteries. This review discusses the interplay between theoretical calculation and experiment in the study of lithium ion battery materials. We introduce the application of theoretical calculation method in solid-state batteries through the combination of theory and experiment. We present the concept and assembly technology of solid-state batteries are reviewed. The basic parameters of solid-state electrolytes, especially sulfide-based solid-state electrolytes and their interface mechanisms with high-voltage cathode materials, are analyzed by theoretical methods. We present an overview on the scientific challenges, fundamental mechanisms, and design strategies for solid-state batteries, especially focusing on the issues of stability on solid-state electrolytes and the associated interfaces with both cathode and electrolyte. Owing to the theoretical models, we can not only reveal the unprecedented mechanism from the atomic scale, but also analyze the interface problems in the battery thoroughly, thus effectively designing more promising electrolyte and interface coating materials. It blazed a new trial for engineering an interphase with improved interfacial compatibility for a long-term cyclability.

  • Zhifeng Li, Qinglong Qiao, Ning Xu, Kai An, Wenchao Jiang, Yi Tao, Pengjun Bao, Yinchan Zhang, Zhaochao Xu
    Chinese Chemical Letters. 2024, 35(2): 108824-.

    Membrane permeability and intracellular diffusion of fluorescent probes determine staining selectivity of intracellular substructures. However, the relationship between the molecular structure of fluorescent probes and their membrane permeability and intracellular distribution is poorly understood. In this paper, we reported a series of 1,8-naphthalimide dyes and carried out cell imaging experiments, and found that the presence of amino hydrogen in these dyes played a crucial role in their cell membrane permeability and intracellular distribution. The secondary amino group containing compounds 1–4 show excellent membrane permeability and strong fluorescence in living cells. While the tertiary amine containing dyes 5 and 6 can hardly permeate the cell membrane though they show extremely similar structure with compounds 2–4. Compound 1 can selectively image lipid droplets by selecting the wavelength of excitation light. With the specificity for lysosomes, 2 and 4 have been used in long-term time-lapses imaging of lysosomal dynamics and tracking the process of lysosome–lysosome interaction, fusion and movement. The effect of hydrogen-containing amino substituent on the cell membrane permeability of fluorescent molecules is promising for the development of better biocompatible probes.

  • Liming Cao, Maolin Sun, Chaoming Liang, Lei Yang, Yueyue Ma, Ruihua Cheng, Yanxiong Ke, Wei Yu, Jinxing Ye
    Chinese Chemical Letters. 2024, 35(2): 108758-.

    Calcium dibutyryladenosine cyclophosphate is a widely used cardiovascular drug. The traditional batch synthesis process suffers from long reaction times, tedious operations, and unstable yields. Herein, a sequential continuous flow synthesis combined with a multistage in-line purification process of calcium dibutyryladenosine cyclophosphate was developed. The acylation reaction was completed in a continuous coil reactor at 160 ℃ in 20 min. And the high toxic solvent pyridine was replaced by acetonitrile. Furthermore, the multistage in-line purification process was integrated into the homemade 3D circular cyclone-type micromixer chip. Combining with the membrane phase separators, the residence time of the purification step was 30 s. The isolated yield of this sequential continuous process was 92% with 99% purity.

  • Yunlei Zhang, Yiran Liu, Wen Guan, Mengxue Cao, Yao Chen, Pengwei Huo
    Chinese Chemical Letters. 2024, 35(2): 108932-.

    The unique properties of metal oxide surfaces, crystal surfaces and defects play vital roles in biomass upgrading reactions. In this work, hierarchical porous bowl-shaped ZrO2 (HB-ZrO2) with mixed crystal phase was designed and employed as the support for loading AuPd bimetal with different proportions to synthesize AuPd/HB-ZrO2 catalysts. The effects of surface chemistry, oxygen defects, bimetal interaction and metal-support interaction of AuPd/HB-ZrO2 on catalytic performance for the selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) were systematically investigated. The Au2Pd1/HB-ZrO2 catalyst afforded a satisfactory FDCA yield of 99.9% from HMF oxidation using O2 as the oxidant in water, accompanied with an excellent FDCA productivity at 97.6 mmol g−1 h−1. This work offers fresh insights into rationally designing efficient catalysts with oxygen-rich defects for the catalytic upgrading of biomass platform chemicals.

  • Yuqi Ren, Hongxu Zhang, Caihong Hao, Qing Chang, Ning Li, Jinlong Yang, Shengliang Hu
    Chinese Chemical Letters. 2024, 35(1): 108225-.

    The chemoselective hydrogenation of structurally diverse nitroaromatics is a challenging process. Generally, catalyst activity tends to decrease when excellent selectivity is guaranteed. We here present a novel photocatalyst combining amino-functionalized carbon dots (N-CDs) with copper selenite nanoparticles (N-CDs@CuSeO3) for simultaneously improving selectivity and activity. Under visible light irradiation, the prepared N-CDs@CuSeO3 exhibits 100% catalytic selectivity for the formation of 4-aminostyrene at full conversion of 4-nitrostyrene in aqueous solvent within a few minutes. Such excellent photocatalytic performance is mainly attributed to the precise control of the hydrogen species released from the ammonia borane by means of light-converted electrons upon N-CDs@CuSeO3. Besides, the defect states at the interface of N-CDs and CuSeO3 enable holes to be trapped for promoting separation and transfer of photogenerated charges, allowing more hydrogen species to participate in catalytic reaction.

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