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  • Jiao Li, Chenyang Zhang, Chuhan Wu, Yan Liu, Xuejian Zhang, Xiao Li, Yongtao Li, Jing Sun, Zhongmin Su
    Chinese Chemical Letters. 2024, 35(6): 108782-.

    Hydrogen evolution electrocatalysts derived from metal-organic crystalline frameworks can inherit the merits of ordered and adjustable structures with high surface area. In this paper, organic-octamolybdate crystalline superstructures (OOCS) with a fixed stoichiometric ratio of Mo8(L)2 and high Mo content (> 40 wt%) were synthesized using flexible ligands with controllable lengths (named as OOCS-1–3). Then, molybdenum carbides coated with carbon layers as electrocatalysts (Mo2C@C-1–3) can be obtained directly from a one-step high-temperature carbonization process using OOCS-1–3 as precursors. As a typical example, Mo2C@C-3 exhibits satisfactory hydrogen evolution activity with a low overpotential of 151 mV (1.0 mol/L KOH) at 10 mA/cm2 and stability for 24 h. The electrocatalytic activity is mainly from the synergistic interactions between the carbon layers and molybdenum carbide species. Furthermore, compared with the initial content of C, N, Mo in OOCS and Mo2C@C, the catalytic activity increases with the N amount. This work makes organic-octamolybdate crystalline superstructures used as general precursors to product high Mo content electrocatalysts applied in energy storage and conversion fields.

  • Tianze Wang, Junyi Ren, Dongxiang Zhang, Huan Wang, Jianjun Du, Xin-Dong Jiang, Guiling Wang
    Chinese Chemical Letters. 2024, 35(6): 108862-.

    Integrating ring-fused modification with π-conjugated extension is an effective approach for designing, synthesizing, and application for novel borondipyrromethene (BODIPY) structures. In this work, based on phenyl[b]-fused BODIPY, we made reasonable modification of the methyl group at 1-site to generate dye NBDP. NBDP possessed near-infrared region (NIR) absorption and emission properties, and the intramolecular charge transfer (ICT) resulted in low fluorescence. Whereas, heat energy is evidently released in the presence of light, which can be exploited for intracellular photothermal therapy via the cell apoptosis process, reducing the inflammatory side-effects induced by necrosis. This research provides a crucial foundation for the novel molecule via BODIPY multi-directional alteration and its potential application in anti-tumor phototherapy.

  • Yihan Zhou, Duo Gao, Yaying Wang, Li Liang, Qingyu Zhang, Wenwen Han, Jie Wang, Chunliu Zhu, Xinxin Zhang, Yong Gan
    Chinese Chemical Letters. 2024, 35(6): 108967-.

    Local delivery of nanoparticles holds promise for colorectal cancer (CRC) therapy. However, the presence of the mucus layer on the epithelium poses a significant challenge to drug delivery, thereby adversely affecting treatment efficiency. It is crucial to develop efficient drug delivery carriers that can effectively overcome mucus barriers to treat colorectal cancer. Herein, we utilized poly(1,4-butadiene)-b-poly(ethylene oxide) polymers to prepare four distinct geometries of polymeric micelles, namely linear micelles (LMs), worm-like micelles (WLMs), large spherical micelles (LSMs), and small spherical micelles (SSMs) to investigate the influence of shape effects on overcoming colonic mucosal barrier. We found that the carriers exhibited diverse shapes while maintaining comparable physicochemical properties. Of these, WLMs had an aspect ratio similar to segmented filamentous bacteria, which exhibited superior mucus penetration ability, leading to prolonged drug release kinetics and faster entry into epithelial cells compared to LSMs. Furthermore, rectally administrated 10-hydroxycamptothecin-loaded WLMs traversed the colorectal mucus in orthotopic CRC nude mice model, penetrated and accumulated within tumor tissue, and effectively aggregated within cancer cells, thereby inducing significantly robust antitumor outcomes in vivo. These findings underscore the significance of shape design in overcoming colonic mucosal absorption barriers, offering a novel approach for the development of drug delivery carriers tailored for effective tumor therapy.

  • Xin Zhang, Junyu Chen, Xiang Pei, Linxin Yang, Liang Wang, Luona Chen, Guangmei Yang, Xibo Pei, Qianbing Wan, Jian Wang
    Chinese Chemical Letters. 2024, 35(6): 108889-.

    Surface modification of microporous bone scaffolds using nanoparticles has been broadly studied in bone tissue engineering. Aiming at improving vascularized bone regeneration (VBR), zeolitic imidazolate framework-8 (ZIF-8) was encapsulated with dimethyloxallyl glycine (DMOG) and the drug-carrying nanoparticles (D@Z) could be uniformly coated onto the surface of the bone scaffold. The osteogenic and angiogenic actions of D@Z are closely correlated with the amount of slowly released DMOG, and in general, exhibited a favorable association. Then, the D7.5@Z group, which showed the greatest capacity to induce in vitro osteogenesis–angiogenesis coupling, was utilized for surface modification of the bone scaffold. Biological processes including phosphate-containing compound metabolic process, cell differentiation, cell proliferation and cell motility might contribute to enhanced ability to induce VBR by the coated scaffold and signaling pathways such as Rap1, Ras, phosphatidylinositol 3-kinase/protein kinase B (PI3K-AKT) and vascular endothelial growth factor (VEGF) signaling pathways participated in these processes. Finally, as depicted by in vitro real time-polymerase chain reaction (RT-PCR), Western blot (WB) and in vivo cranial bone defect model, the microporous scaffold coated with nano-D7.5@Z greatly promoted VBR. To conclude, nano-D@Z has significant promise for practical application in modification of microporous bone scaffolds to enhance VBR, and DMOG loading quantity has a beneficial influence on D@Z to improve osteogenesis–angiogenesis coupling.

  • Jia-Mei Qin, Xue Li, Wei Lang, Fu-Hao Zhang, Qian-Yong Cao
    Chinese Chemical Letters. 2024, 35(6): 108925-.

    A new aggregation-induced emission (AIE)-based fluorescence sensor, TPEPy-SS-C14, for simultaneous recognition of adenosine triphosphate (ATP) and hydrogen sulfide (H2S) has been reported via the aggregation-disaggregation mechanism. The probe self-assembles nano-structure aggregations in aqueous solution. It shows fluorescence turn-on response toward ATP for the complexation-enhanced aggregation, but leads to fluorescence quenching of H2S for cleavage the aggregations.

  • Guihuang Fang, Wei Chen, Hongwei Yang, Haisheng Fang, Chuang Yu, Maoxiang Wu
    Chinese Chemical Letters. 2024, 35(6): 108799-.

    The addition of electrolyte additives is an effective strategy for tuning the property of the electrolyte to engineer the electrode/electrolyte interface, and there exist obvious discrepancies regarding the effect of fluoroethylene carbonate (FEC) as an electrolyte additive on the performance of cathodes. Herein FEC is introduced into the electrolyte of the LiMn0.8Fe0.2PO4/Li cell and its effect on the properties of the LiMn0.8Fe0.2PO4 is investigated. It is found that the addition of FEC in the electrolyte has a positive effect on the performance of the LiMn0.8Fe0.2PO4 cathode, which can be attributed to the reduced products generated by the interfacial side-reactions on the LiMn0.8Fe0.2PO4 cathode surface and the decreased metal dissolution in the FEC-containing electrolyte, thanks to the higher oxidation resistance of FEC and the easier and stronger binding of FEC and PF6.

  • Zhongjie Li, Xiangyue Kong, Yuhao Liu, Huayu Qiu, Lingling Zhan, Shouchun Yin
    Chinese Chemical Letters. 2024, 35(6): 109378-.

    The microstructure of the active layer in organic photovoltaics (OPVs), such as the size of phase separation, purity of the phases, and molecular packing within each phase, plays a crucial role in influencing the behavior of excitons and charge carriers within the active layer. It is also a key determinant of the photovoltaic performance of the device. During the optimization of OPV devices, the use of additives has been demonstrated to be an effective strategy in microstructure control, leading to enhanced performance. Therefore, the quest for stable and efficient novel additives, along with an exploration and summarization of the mechanisms underlying additive-induced microstructure control, is essential for a better understanding of the developmental trends of high-performance additives. In this review, we categorize additives based on their chemical structures and discuss their effects on the microstructure of the active layer from both thermodynamic and kinetic perspectives. Furthermore, we elaborate on the working mechanisms and their impact on the photovoltaic performance of the devices. This review provides an overview of recent advances in additives for OPVs, offering potential guidance for the future development of additives and further optimization of the active layer in photovoltaic devices.

  • Jia-Li Xie, Tian-Jin Xie, Yu-Jie Luo, Kai Mao, Cheng-Zhi Huang, Yuan-Fang Li, Shu-Jun Zhen
    Chinese Chemical Letters. 2024, 35(6): 109137-.

    Fluorescence Anisotropy (FA) is an effective biochemical detection method based on molecular rotations. Graphene oxide (GO) has been extensively used as an FA amplifier. However, the enhancement of FA by GO alone is limited and the strong scattering of GO will easily make the measurement of FA inaccurate. In order to address these problems, an octopus-like DNA nanostructure (ODN) was designed and coupled with GO to enhance the FA together in this work. By mimicking the multi-clawed structure of the octopus, the ODN can be adsorbed on GO tightly, which not only could improve the sensitivity because of the double FA enhancement abilities of GO and ODN, but also could improve the specificity due to the decrease of the nonspecific interaction in complex samples. Furthermore, ODN could maintain a certain distance between the fluorophore and GO to reduce the fluorescence quenching efficiency of GO, which could improve the accuracy. This method has been applied for the detection of hepatitis B virus DNA (HBV-DNA) in a range of 1–50nmol/L and the limit of detection (LOD) was 330pmol/L. In addition, the proposed method has been successfully utilized to detect HBV-DNA in human serum, indicating that this method has a great practical application prospect.

  • Huan Yao, Jian Qin, Yan-Fang Wang, Song-Meng Wang, Liu-Huan Yi, Shi-Yao Li, Fangfang Du, Liu-Pan Yang, Li-Li Wang
    Chinese Chemical Letters. 2024, 35(6): 109154-.

    Artificial macrocycle with high binding selectivity in water is often challenging but urgently needed in various research and application areas. Herein, we report a new water-soluble biomimetic tetralactam macrocycle and realize the ultra-high selectivity to nucleosides over corresponding monophosphate nucleotides by rational modification. The introduction of charged groups at the periphery of endo-functionalized cavity makes the selectivity (guanosine to guanosine 5′-monophosphate) increase remarkably from 100 to 1119. Based on the ultra-high selectivity of biomimetic tetralactam macrocycle, the sensitive CD73 enzyme activity assay was then achieved through product-selective fluorescence indicator displacement assay. Furthermore, the capability of the proposed method for inhibitor screening was successfully displayed.

  • Gengchen Guo, Tianyu Zhao, Ruichang Sun, Mingzhe Song, Hongyu Liu, Sen Wang, Jingwen Li, Jingbin Zeng
    Chinese Chemical Letters. 2024, 35(6): 109198-.

    Lateral flow immunoassay (LFIA) has become popular in laboratories, at-home testing, and medical diagnostics due to its minimal cost and user-friendliness. Nevertheless, conventional test strips based on colloidal gold can only obtain qualitative or semi-quantitative results with low sensitivity. In this work, Au-Fe3O4 dumbbell-like nanoparticles were synthesized and used as the LFIA labelling marker for highly sensitive colorimetric-photothermal dual-mode detection of SARS-CoV-2 spike(S) protein. The unique dumbbell structure of Au-Fe3O4 NPs makes it possible to combine the best features of both Au NPs and Fe3O4 NPs. The increased surface area of these NPs enhances their LSPR effect and photothermal effect, which achieves signal amplification to increase sensitivity. The Au-Fe3O4 NPs modified with S protein antibody could identify S protein in samples, which were recognized and accumulated on T-line by another antibody, generating color band for qualitative colorimetric detection. The T-line was irradiated by laser to obtain temperature change for quantitative detection of photothermal. In optimized conditions, the detection limit was 1.22 pg/mL, three orders of magnitude more sensitive than colorimetric detection. Finally, the approach was performed on SARS-CoV-2 pseudovirus samples and outperformed traditional colloidal gold strips. This LFIA platform exhibits significant promise for practical implementation, as it can satisfy the need for low-cost, high-sensitivity, and home-based quantitative detection for respiratory infectious diseases.

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