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  • Ya Song, Mingxia Zhou, Zhu Chen, Huali Nie, Jiao-Jing Shao, Guangmin Zhou
    Chinese Chemical Letters. 2024, 35(6): 109200-.

    The practical application of high-energy-density lithium-sulfur (Li-S) batteries have been highly praised for energy storage devices, while are largely hindered by the "shuttling effect". Herein, core-shell carbon spheres composed of interlinked porous core and lamellar shell were designed to restrain the polysulfide shuttling. The microporous structure with pore size of around 1 nm effectively trap lithium polysulfides. Furthermore, the interconnected porous core shortens the ion transfer distance and the lamellar carbon shell endows the carbon spheres with fast electron conduction, finally facilitating polysulfide conversion kinetics. Therefore, the Li-S batteries with the carbon spheres as the interlayer show high discharge specific capacity of 1002 mAh/g at 2 C with 574 mAh/g remaining after 600 cycles, and high areal capacity of 5.48 mAh/cm2 with sulfur loading of 4.67 mg/cm2 at 0.1 C. The corresponding pouch cells also exhibit stable cycling stability with an initial discharge specific capacity of 1082 mAh/g at 0.1 C.

  • Huizhong Wu, Ruiheng Liang, Ge Song, Zhongzheng Hu, Xuyang Zhang, Minghua Zhou
    Chinese Chemical Letters. 2024, 35(6): 109131-.

    To mitigate the water pollution problem by photocatalytic degradation of typical antibiotics of tetracycline (TC), we prepared defective Bi2Sn2O7 (BSO) quantum dots (QDs) with a full spectral response due to Bi metal deposition, using a one-pot hydrothermal method, labeled as Bi@BSO-OV. The optimized Bi@BSO-OV showed 73.4% removal of TC in 1 h under irradiation with a 50 W LED lamp in the wavelength band in the visible-near-infrared (vis-NIR) light, a rate that is substantially greater than that of pure BSO (14.7%). The synergistic interaction of Bi metal and oxygen vacancies (OVs) is crucial to boosting photocatalytic performance. The near-infrared region of the photo-response is extended by the surface plasmon resonance (SPR) effect of Bi metal, enhancing the photocatalytic performance and dramatically raising the efficiency of solar energy utilization. In addition to inducing defect levels in BSO, the OVs also activate the surface adsorbed O2 to promote the production of O2 and 1O2. DFT calculations reveal that Bi metal and OVs can mutually tune the charge transfer pathways. On the one hand, Bi metal can act as both a charge transfer bridge and an electron donor to assist charge separation. On the other hand, OVs-induced defect levels allow electrons that leap to the conduction band (CB) to first leap from the valence band (VB) to the defect levels, notably improving interfacial charge separation and transfer. The concept of design executed in this study for altering the catalyst by introducing both OVs and Bi metal can provide a rational design idea and potential insight for improving the photocatalytic activity for environmental applications.

  • 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.

  • 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.

  • Xin-Tong Zhao, Jin-Zhi Guo, Wen-Liang Li, Jing-Ping Zhang, Xing-Long Wu
    Chinese Chemical Letters. 2024, 35(6): 108715-.

    Nowadays, lithium-ion batteries (LIBs) play a crucial role in modern society in the aspect of portable electronic devices and large-scale smart grids. However, the current performance of lithium-ion batteries has been unable to meet the growing expectations of society and scientific community. Herein, we have synthetically investigated availability of 2D Ni-TABQ monolayer as anode based on DFT for LIBs applications. Our findings have demonstrated that 2D Ni-TABQ monolayer is a semiconductor with a small band gap of 0.2 eV, which suggest that the electronic property of 2D Ni-TABQ monolayer would take place an evident shift from semiconductor property to metallic property after Li adsorption. Furthermore, we checked the stability of 2D Ni-TABQ monolayer and investigated the viability of exfoliation from bulk multilayer Ni-TABQ to form 2D Ni-TABQ monolayer in the light of exfoliation energy and binding energy. We continuously studied electrochemical properties of 2D Ni-TABQ monolayer with respect of theoretical specific capacity, Li-ion diffusion barriers and open-circuit voltage. During the charging process, 2D Ni-TABQ monolayer can achieve a high specific capacity of 722 mAh/g with an open-circuit voltage range from 1.12 V to 0.22 V. These aforementioned results make the 2D Ni-TABQ monolayer a promising anode for LIBs.

  • 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.

  • Xing Tian, Di Wu, Wanheng Wei, Guifu Dai, Zhanxian Li, Benhua Wang, Mingming Yu
    Chinese Chemical Letters. 2024, 35(6): 108912-.

    Abnormal accumulation and metabolism of lipid droplets can lead to a variety of diseases. Polarity, a key parameter of the microenvironment, is closely associated with many diseases and dysfunctions in the body. It is important to elucidate the relationship between the physiological activity of lipid droplets (LDs) and the polarity of the microenvironment. In this work, based on push-pull mechanism, a fluorescent probe (E)-3-(5-(4-(diphenylamino)phenyl)thiophen-2-yl)-1-(2-hydroxyphenyl)prop-2-en-1-one (PPTH) with aggregation-induced emission (AIE) properties for the detection of polarity changes in cells was synthesized. PPTH not only visualize intracellular polarity fluctuation of iron death and inflammation but also distinguish between normal and fatty liver tissue.

  • 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.

  • Qianqian Song, Yunting Zhang, Jianli Liang, Si Liu, Jian Zhu, Xingbin Yan
    Chinese Chemical Letters. 2024, 35(6): 108797-.

    Polyethylene oxide (PEO)-based solid-state polymer electrolytes (SPEs) are limited by their poor cyclic stability and inferior ionic conductivity for applicating in high-safety, long-cycling and high-energy-density lithium metal batteries. Herein, porous boron nitride nanofibers (BNNFs) are filled into PEO-based SPE, which significantly suppresses Li dendrites growth and enhances the electrochemical performance of Li metal battery. BNNFs with high porosity have more active sites to connect with PEO, which can effectively reduce the crystallinity of the PEO matrix and enhance its ionic conductivity. Moreover, owing to the hardness and good stability of BNNFs, BNNFs/PEO/LiTFSI electrolyte exhibits a wider electrochemical window, better mechanical property and higher thermal stability compared with PEO/LiTFSI electrolyte. Consequently, the Li symmetric cell composed of 1% BNNFs/PEO/LiTFSI performs good cyclic stability (>1800 h), and the Li||1% BNNFs/PEO/LiTFSI||LFP full battery shows obviously improved performances in charge-discharge polarization voltage, discharge specific capacity, rate performance and cyclic stability than the Li||PEO/LiTFSI||LFP battery.

  • Hualei Xu, Manman Han, Haiqiang Liu, Liang Qin, Lulu Chen, Hao Hu, Ran Wu, Chenyu Yang, Hua Guo, Jinrong Li, Jinxiang Fu, Qichen Hao, Yijun Zhou, Jinchao Feng, Xiaodong Wang
    Chinese Chemical Letters. 2024, 35(6): 109095-.

    Low-molecular-weight (LMW) compounds are ubiquitous in living organisms and play essential roles in biological processes. The direct analysis of LMW compounds in biological tissues by matrix-assisted laser desorption/ionization mass spectrometry imaging (MALDI-MSI) could provide a more comprehensive understanding of their essential functions. Here, we evaluated 4-nitrocatechol (4-NC) as a novel positive-ion matrix for enhancing in situ detection and imaging of LMW compounds from the rat liver, brain, and germinating Chinese-yew seed by MALDI-MS. Our results showed that the 4-NC possessed remarkable features, including strong ultraviolet absorption, uniform matrix crystal, excellent chemical stability, and fewer matrix-related background peaks. The use of 4-NC led to the successful detection of 232, 218, and 193 LMW compounds from the three abovementioned tissue sections, respectively. Also, the use of 4-NC improved the imaging quality of LMW compounds in tissue sections through MALDI-MSI and has the potential as a matrix for MALDI tissue imaging of LMW compounds.

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