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  • Jing Guo, Ruichen Shen, Xuejie Shen, Bo Zeng, Nianjun Yang, Huageng Liang, Yanbing Yang, Quan Yuan
    Chinese Chemical Letters. 2022, 33(2): 979-982.

    Bladder cancer is the most common malignant tumours with high morbidity, mortality and recurrence. However, currently developed detection methods for bladder cancer-associated urine biomarkers are hindered by their extremely low abundance. Hence, the exploration of a highly sensitive and selective approach for the detection of trace bladder cancer-associated biomarkers in human urine is of vital importance for the diagnosis of bladder cancer. Herein, we developed a highly reliable indium gallium zinc oxide field effect transistor (IGZO FET) biosensor for the detection of bladder cancer-related biomarker microRNA. The single-stranded DNA-functionalized IGZO FET biosensors exhibit high sensing reproducibility and stability with an ultralow detection limit of 19.8 amol/L. The device could also be used for quantitative detection of trace microRNA in human urine samples and can effectively distinguish bladder cancer patients from healthy donors. The development of high performance IGZO FET biosensors presents new opportunities for the achievement of early-stage diagnosis of bladder cancer.

  • Maoju Chang, Chenxu Yan, Lei Shi, Dan Li, Wei Fu, Zhiqian Guo
    Chinese Chemical Letters. 2022, 33(2): 762-766.

    Cysteine is well-known to be an important biothiol and related to many diseases. However, the in vivo detection of endogenous cysteine still suffers from lacking small-molecule fluorophores with both excitation and emission in the near-infrared (650-900 nm)/shortwave-infrared region. Herein, we report a molecular engineering strategy for shortwave infrared (SWIR, 900-1700 nm) sensing of cysteine, which integrated an excited-state intermolecular proton transfer (ESIPT) building block into the intramolecular charge transfer (ICT) scaffold. The obtained novel fluorophore SH-OH displays a maximum absorption at the NIR region, and emission at the SWIR region. We introduce the cysteine-recognition moiety to SH-OH structure, and demonstrate sensing of endogenous cysteine in living animals, using the SWIR emission as a reliable off-on fluorescence signal. This fluorophore design strategy of cooperation of ICT and ESIPT processes expands the in vivo sensing toolbox for accurate analysis in clinical applications.

  • Yinghua Niu, Weirong Huo, Yuandong Yu, Wenjun Li, Yulin Chen, Weiqiang Lv
    Chinese Chemical Letters. 2022, 33(2): 674-682.

    To lower the operation temperature and increase the durability of solid oxide fuel cells (SOFCs), increasing attentions have been paid on developing cathode materials with good oxygen reduction reaction (ORR) activity at intermediate-temperature (IT, 500–750 ℃) range. However, most cathode materials exhibit poor catalytic activity, or they thermally mismatch with SOFC electrolytes and undergo severe degeneration. Infiltrating catalysts on existing backbone materials has been proved to be an efficient method to construct highly active and durable cathodes. In this mini-review, the advantages of infiltration-based cathode compared with new material-based cathodes are summarized. The merits and drawbacks of different backbones are illustrated. Different types of catalysts for infiltration are depicted in detail. Suggestions on the material/structure optimization of the infiltrated cathodes of IT-SOFC are provided.

  • Longmei Li, Jin Zhang, Wenjing Sun, Weimin Gong, Changlin Tian, Pan Shi, Chaowei Shi
    Chinese Chemical Letters. 2022, 33(2): 747-750.

    Current resolved structures of GPCRs and G protein complexes provided important insights into G protein activation. However, the binding or dissociation of GPCRs with G protein is instantaneous and highly dynamic in the intracellular environment. The conformational dynamic of G protein still needs to be addressed. In this study, we applied 19F solution NMR spectroscopy to monitor the conformational changes of G protein upon interact with detergent mimicking membrane and receptor. Our results show that there are two states equilibria in the Gα in apo states. The interaction of Gα with detergents will accelerate this conformational transformation and induce a state that tends to bind to GPCRs. Finally, the Gα proteins presented a fully activation state when they coupled to GPCRs.

  • Huimin Liu, Qinglei Liu, Yarong Wang, Yongfei Wang, Shulei Chou, Zhizhi Hu, Zhiqiang Zhang
    Chinese Chemical Letters. 2022, 33(2): 683-692.

    Efficient bifunctional OER/ORR catalysts are crucial for the further development of zinc-air battery. From a sustainable point of view, it is important that electrocatalysts are efficient, low cost, and composed of abundant resources instead of scarce metals. Due to their good conductivity, low cost, and strong durability, carbon-based materials are considered a promising alternative in the field of commercial zinc-air battery catalysts. Herein, we briefly introduce the zinc-air battery and then summarize recent progress in the development of carbon-based bifunctional catalysts by defect engineering, heteroatom doping and metal doping. Finally, we discuss the main challenges and prospects for the future development of carbon-based bifunctional oxygen catalysts.

  • Yuejia Song, Yaqian Huang, Fang Zhou, Jinsong Ding, Wenhu Zhou
    Chinese Chemical Letters. 2022, 33(2): 597-612.

    Macrophage is the key innate immune effector in first-line defense against the pathogens, and can be polarized into different phenotypes to regulate a variety of immunological functions. However, the plasticity of macrophage is extraordinarily recruited, activated, and polarized under pathological conditions, playing paramount roles in occurrence, development, and prognosis of various chronic diseases, such as rheumatoid arthritis (RA), atherosclerosis (AS), and cancer. To this end, macrophage has become an important therapeutic target for etiological treatment of these diseases. Meanwhile, with the development of nanotechnology, various nano-drug delivery systems have been explored to target macrophages for disease modulation, displaying unique advantages to address both pharmaceutic and biopharmaceutic limitations of various drugs. This review aims to summarize the recent progress of macrophage-targeted nanomedicine for chronic diseases immunotherapy. First, the origin, polarization and biological functions of macrophages have been introduced, in which macrophages can differentiate into different phenotypes in response to physiological stimuli to play various immunological roles. Then, the macrophage disorder has been reviewed in related with various chronic diseases, and several representative diseases, including AS, RA, obesity, and cancer, have been discussed in detail to elucidate the pathological contributions of macrophages for disease progress. Next, strategies to regulate macrophages for diseases immunotherapy, such as macrophages depletion, macrophage reprograming, inhibition of macrophage recruitment, are summarized, and particular attention has been paid on bio-functional nanomaterials to engineer macrophages via different mechanisms. Further, methods for macrophage-targeting delivery nanosystems are discussed based on both passive and active targeting approaches. Finally, the perspective is speculated for potential clinical translation, and there still has significant room for the development of novel macrophage-targeting nanomedicine for precise, effective, and biosafe therapy.

  • Bingxin Wu, Fanglin Du, Wenjing A, Guofeng Li, Xing Wang
    Chinese Chemical Letters. 2022, 33(2): 703-713.

    Graphene-based sponge is a novel hemostatic material prepared by chemical cross-link of graphene oxide. It has a fast fluid absorption capacity to quickly absorb blood from wounds, activate clotting pathways, and achieve rapid hemostasis. In addition, graphene-based sponge is also a good platform carrier. It can be prepared by organic cross-linking, compounding with inorganic clay, and adding bioactive factors to enhance coagulation stimulation. By these methods, the hemostatic performance of the sponge is further improved, which shows great potential for application in the field of trauma hemostasis. This article reviews the research progress of graphene-based sponges from three different preparation strategies (organic cross-linking, inorganic compounding and adding bioactive factor), summarizes their hemostatic mechanisms, and prospects the development of graphene-based hemostatic sponges.

  • Yutian Qin, Yue Wan, Jun Guo, Meiting Zhao
    Chinese Chemical Letters. 2022, 33(2): 693-702.

    As emerging two-dimensional materials, metal-organic framework (MOF) nanosheet composites possess many unique physical and chemical properties, thus being expected to be widely applied in gas separation and adsorption, energy conversion and storage, heterogeneous catalysis, sensing as well as biomedicine. In this review, we first introduce the methods for integrating MOF nanosheets with other materials to prepare multifunctional composites. Next, the applications of MOF nanosheet composites in versatile fields are summarized and discussed. We hope this review will be instructive for researchers in the aspects of designs, preparations and applications of MOF nanosheet composites.

  • Jianhua Yan, Yixuan Zhang, Lijuan Zheng, Yuwei Wu, Ting Wang, Ting Jiang, Xiaoqin Liu, Dongming Peng, Yanfei Liu, Zhenbao Liu
    Chinese Chemical Letters. 2022, 33(2): 767-772.

    The drug resistance of chemotherapy is a major challenge to overcome for antineoplastic agents and the reverse of drug resistant is essential for cancer therapy. Herein, we developed a drug delivery system which can simultaneously detect/reverse the drug resistance and perform synergetic treatment of cancer. In this work, we integrated cyanine5 (Cy5) modified miRNA (let-7i) (Cy5-miRNA) and platinum onto nano-graphene oxide (NGO) (30-50 nm) platform to achieve simultaneously detection/reversion of drug resistance and synergetic treatment of cisplatin resistant SKOV3 cells (SKOV3DDP cells). The Cy5-miRNA adsorbed on NGO could selectively bind the drug resistance related mRNA follow by suppress the expression of drug resistance mRNA, and the binding simultaneously induced the release of Cy5-miRNA from the NGO, thus the fluorescence signal of Cy5 recovered and could be used for drug resistance monitoring. Moreover, the miRNA suppressed the Cyclin D1 protein expressions thus reversed the drug resistance. The loaded platinum(IV) (Pt(IV)) was converted to the therapeutic platinum(II) (Pt(II)) in both tumor acidic and reductive environment responsive behavior. NGO furtherly performed photothermal therapy under near infrared (NIR) laser irradiation and enhanced the therapeutic effect. All in all, this nanoplatform realized detection/reversion of the drug resistance as well as synergetic chemical-photothermal treatment of ovarian cancer cells, which holds great promise in the treatment of drug resistant cancer cells.

  • Qiuying Du, Baoqi Yin, Si Zhou, Zhixun Luo, Jijun Zhao
    Chinese Chemical Letters. 2022, 33(2): 995-1000.

    The activation of molecular oxygen is an important step in metal-catalyzed oxidation reactions and a hot subject for the research of gas-phase metal clusters. It is known that the Ag and Au clusters readily react with O2 when they have open shell electronic structures. Distinct from this, here we observed Cun (n = 7−20) clusters of both open and closed shells possess high reactivity with O2 with few exceptions. In a combination with ab initio calculations, we demonstrate that the activation of O2 on the even- and odd-sized Cun clusters follows the single and double electron transfer models, respectively. Such phenomenon of metal clusters with different basicity to activate oxygen is enabled by the leveling effect of spin accommodation. The activity of Cun clusters is correlated to the HOMO level, and for the close-shell clusters is also governed by the vertical spin excitation energy (VSE). In encountering the attack of dioxygen, the activity of the copper cluster anions not only depends on their basicity to donate electrons, but also closely associated with the cluster sizes. Small copper clusters Cun (n = 7−13) can dissociate O2 spontaneously, while large clusters require extra energies and display close relationship between the reaction rates and electronic vertical detachment energies (VDE). Our work illuminates a novel reaction mechanism between Cun clusters and O2, which sheds light in manipulating the activity and stability of coinage clusters by controlling the spin and charge states.

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