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  • Shan Jiang, Lingchen Meng, Wenyue Ma, Qingkai Qi, Wei Zhang, Bin Xu, Leijing Liu, Wenjing Tian
    Chinese Chemical Letters. 2024, 35(12): 108998-.
  • Jiahao Liu, Peng Liu, Junhong Duan, Qiongxuan Xie, Jie Feng, Hongpei Tan, Ze Mi, Ying Li, Yunjie Liao, Pengfei Rong, Wenhu Zhou, Xiang Gao
    Chinese Chemical Letters. 2024, 35(12): 109632-.

    Radiotherapy (RT) is a widely used cancer treatment, and the use of metal-based nano-radiotherapy sensitizers has shown promise in enhancing its efficacy. However, efficient accumulation and deep penetration of these sensitizers within tumors remain challenging. In this study, we present the development of bismuth/manganese biomineralized nanoparticles (BiMn/BSA) with multiple radiosensitizing mechanisms, including high atomic number element-mediated radiation capture, catalase-mimic oxygenation, and activation of the stimulator of interferon genes (STING) pathway. Significantly, we demonstrate that low-dose RT induces the recruitment of macrophages and subsequent upregulation of Matrix metalloproteinases (MMP)-2 and MMP-9 that degrade the extracellular matrix (ECM). This dynamic process facilitates the targeted delivery and deep penetration of BiMn/BSA nanoparticles within tumors, thereby enhancing the effectiveness of RT. By combining low-dose RT with BiMn/BSA nanoparticles, we achieved complete suppression of tumor growth in mice with excellent biocompatibility. This study provides a novel and clinically relevant strategy for targeted nanoparticle delivery to tumors, and establishes a safe and effective sequential radiotherapy approach for cancer treatment. These findings hold great promise for improving the outcomes of RT and advancing the field of nanomedicine in cancer therapy.

  • Ziyou Zhang, Te Ji, Hongliang Dong, Zhiqiang Chen, Zhi Su
    Chinese Chemical Letters. 2024, 35(12): 109542-.

    The usage of flexible ligands in constructing MOF materials (FL-MOFs) has been widely studied due to its numerous advantages, including the structural diversity, polynuclear MOFs, transmitting magnetic exchanges, enantioselective separation, asymmetric catalysis, etc. However, the field still faces challenges in deeply understanding the effect of ligand configuration on the properties of these materials. Here, we employ a flexible aggregation-induced emission ligand (4,4′-((1E, 1′E)-anthracene-9,10-diylbis(ethene-2,1-diyl))dibenzoic acid) with great mechanical stability to construct FL-MOFs to lock the ligand configuration to explore the pressure-induced evolution of the ligand with coordination restriction, involving changes in fluorescence and intermolecular interaction. In-situ high-pressure fluorescence, Raman, and FT-IR experiments have revealed that the intermolecular interaction of AIE-Mn-MOF with configuration restriction increased more rapidly than that of free AIE-L. This discovery offers valuable insights for synthesizing MOF materials with exceptional mechanical stability and significantly advances our understanding of the impact of coordination restriction in FL-MOFs on their response to external stimuli.

  • Mao-Fan Li, Ming‐Yu Guo, De-Xuan Liu, Xiao-Xian Chen, Wei-Jian Xu, Wei-Xiong Zhang
    Chinese Chemical Letters. 2024, 35(12): 109507-.

    Multi-stimuli responsive materials controlled and coupled by two or more channels have a broad range of applications in the field of switches, memories, and molecular machines. The exploration of the material is currently focused on the pure organic system, which limits the development of such materials greatly. In this work, we present a new chiral organic-inorganic hybrid salt, (R-3-hydroxypyrrolidinium)2[Fe(CN)5(NO)] (1), which exhibits rare multi-stimuli responsive behaviors in thermal, mechanical and optical channels. In detail, 1 undergoes a C2-P21221 phase transition deriving from the thermal motion of organic cations with the increase of temperature, but the reverse transition can only be induced by mechanical pressure. Moreover, polycrystalline hybrid salt showed photo-responsive performance, i.e., the ground-state N-bound nitrosyl ligand adopts two configurations in excited states caused by light in 532 nm irradiation, accompanying with a photo-induced structural transformation of the anionic framework. Namely, the thermal motion characteristics of organic cations, the photoresponse characteristics of anionic inorganic skeleton and the pressure characteristics from hydrogen bonds are simultaneously integrated in 1. This unprecedented coupling mechanism of multi-stimuli responses makes 1 a potential candidate for future multichannel data storage applications.

  • Shaoming Dong, Yiming Niu, Yinghui Pu, Yongzhao Wang, Bingsen Zhang
    Chinese Chemical Letters. 2024, 35(12): 109525-.

    Control of subsurface interstitial atoms in transition metals is an effective approach to modulate selectivity in hydrogenation reactions. In this study, nickel was alloyed with gallium to form Ni3Ga, thereby regulating the octahedral interstitial sites. Subsequently, carbon atoms were introduced into the Ni3Ga (forming Ni3GaC0.5) via thermal treatment in an acetylene atmosphere, leading to a significant enhancement in selectivity for acetylene hydrogenation reaction. The X-ray diffraction and transmission electron microscopy results demonstrate an increase in the lattice parameter due to the incorporation of carbon atoms and the uniform distribution of carbon in Ni3GaC0.5 nanoparticles. The obtained Ni3GaC0.5/oCNT catalyst exhibits significantly improved selectivity in acetylene hydrogenation reaction, with approximately 82% ethylene selectivity at 98% conversion. Furthermore, it maintains good selectivity at various hydrogen-to-alkyne ratios and displays good stability during long-term operation. The introduction of carbon suppresses the formation of the subsurface hydrogen structure under reaction conditions. Additionally, the charge transfer between carbon and nickel results in the electron deficiency of nickel, effectively inhibiting the over-hydrogenation pathway and enhancing the selectivity. These results provide insights for the design of non-precious metal catalysts in selective hydrogenation reactions.

  • Xiangkang Jiang, Zhixing Wang, Hong Dong, Xiang Zhang, Jin Hu, Manman Chu, Yanshuai Hong, Lei Xu, Wenjie Peng, Xiqian Yu, Jiexi Wang
    Chinese Chemical Letters. 2024, 35(12): 109553-.

    The increasing demand for energy density pushes LiCoO2 (LCO) to work at higher voltage (≥4.5 V), which brings a series of problems including detrimental phase transition and structural instability. Various elemental doping has been proven an effective strategy to improve its structure stability. However, the understanding of elemental doping homogeneity effect is not enough, whether in terms of the controllability of doping homogeneity or its complex consequences. In this work, LCO powders with different Al doping homogeneity were synthesized and tested under high voltage (≥4.5 V) in both half and full cell at room and high temperature, respectively. The results show that the Al homogeneously doped LCO showed better cycling stability and rate performance compared to the inhomogeneous LCO sample. Particularly, the discharge capacity of Al homogeneously doped LCO after 500 cycles under 4.5 V in full cells could reach 160.1 mAh/g at 1.0 C with 94.1% capacity retention. Postmortem characterization demonstrates that a better doping homogeneity favors the stability of both the bulk and interface as well as the kinetic conditions. This study provided new insights about LCO performance fading, which sheds new light on the development of high-voltage LCO products

  • Jiaxu Wang, Jinxie Zhang, Xiuping Wang, Jingying Wang, Lina Chen, Jiahui Cao, Wei Cao, Siyu Liang, Ping Luan, Ke Zheng, Xiao-Kun Ouyang, Li Gao, Xiaowen Ou, Fan Zhang, Meitong Ou, Lin Mei
    Chinese Chemical Letters. 2024, 35(12): 109697-.

    The utilization of fungicides in plants is very low, emphasizing the need to improve their utilization rates. In this study, the fungicide dimethachlon (Dim) was encapsulated within hollow mesoporous silica (HMSNs), and a coating was formed on the HMSNs surface through the reaction of Na2CO3 and CaCl2, resulting in a pH-responsive delivery system named D/H@CaCO3, proven valuable in preventing sclerotinia diseases in romaine lettuce. When disease-infested romaine lettuce was treated with D/H@CaCO3, it degraded in the acidic microenvironment of Sclerotinia sclerotiorum (S. sclerotiorum), allowing for the pH-responsive release of Dim and effectively killing S. sclerotiorum. Moreover, the degraded CaCO3 coating releases CO2, which enhances the photosynthetic pigment contents, such as chlorophyll a, chlorophyll b, and carotenoids, in turn promoting plant growth. D/H@CaCO3 is biologically safe for plants and is environmentally friendly, as confirmed by assessments involving zebrafish and earthworms. Given their antifungal capabilities, the controlled release of fungicides offers potential for plant protection.

  • Wenhao Feng, Chunli Liu, Zheng Liu, Huan Pang
    Chinese Chemical Letters. 2024, 35(12): 109552-.

    Graphene-like materials and metal-organic framework (MOF) materials hold significant promise for advanced energy systems. However, the accumulation of two-dimensional (2D) material and the low conductivity of MOF have seriously affected their practical application. The universal method for synthesizing homogeneous nitrogen-doped graphene-like carbon/metal-organic framework (N-GLC/MOF) composites, including N-GLC/MOF-74, N-GLC/ZIF-8, N-GLC/Cu-BTC, and N-GLC/FeCo-PBA was presented. Thanks to the synergistic effect of the two components, the N-GLC/MOF-74 composite exhibits a specific capacitance of 470.18 F/g at 1 A/g and maintains a coulombic efficiency of 95.04% at 5 A/g over 5500 cycles. Our work lays a solid foundation for the design and synthesis of N-GLC-based composites. We anticipate that this research will furnish valuable insights for the advancement of N-GLC/MOF composites, with a primary focus on enhancing supercapacitor performance.

  • Qihang Wu, Hui Wen, Wenhai Lin, Tingting Sun, Zhigang Xie
    Chinese Chemical Letters. 2024, 35(12): 109692-.

    Photodynamic therapy has been widely employed as an alternative strategy against bacterial infection. Molecular structure has a profound effect on the antibacterial ability of photosensitizers (PSs). Herein, we designed and synthesized a series of boron dipyrromethene (BODIPY)-based photosensitizers with different alkyl chain lengths, and then their antibacterial activities were compared. Among these BODIPYs, the BODIPY with octyl (BDP-8) exhibits the best antibacterial effect, while the antibacterial performance of BODIPY with dodecyl (BDP-12) is the worst. This work provides instructive information for further development of effective photodynamic antimicrobial agents.

  • Mengyuan Li, Xitong Ren, Yanmei Gao, Mengyao Mu, Shiping Zhu, Shufang Tian, Minghua Lu
    Chinese Chemical Letters. 2024, 35(12): 109699-.

    In view of widespread existence and toxicity, removal and detection of bisphenols is imperative to assess environmental risks and reduce harm to human health. Although many techniques have been reported, constructing fast and sensitive method remains a challenge. Herein, porous poly(divinylbenzene) polymer was synthesized in-situ on the Fe3O4 particles by means of distillation-precipitation polymerization and functioned as sorbents to extract bisphenols. Employing Fe3O4@poly(divinylbenzene) as sorbent, a magnetic solid-phase extraction coupling with liquid chromatography was developed to detect trace bisphenols in water. This method presented low detection limits (0.01–0.03 ng/mL), high enrichment ability (enrichment factor, 327–343), and good reproducibility. Moreover, the method showed satisfactory recoveries in the detection of lake water (80.60%-116.2%) and egg sample (75.17%-120.0%). Impressively, Fe3O4@PDVB has excellent adsorption capacity, which can realize rapid kinetic adsorption of bisphenols with equilibrium time all less than 10 s. The maximum adsorption capacities reached 1074.8, 1049.7, 1299.1 and 1329.5 mg/g for bisphenol F, bisphenol A, bisphenol B and bisphenol AF with Langmuir isotherm model. The adsorption mechanism of Fe3O4@PDVB to bisphenols was investigated and demonstrated that hydrophobic interactions played a key role, together with assistance of stacking interactions and hydrogen interactions. Overall, this work provides a promising sorbent material with ultra-fast and large adsorption capacities for extraction of bisphenols from water.

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