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  • Mingjiao Lu, Zhixing Wang, Gui Luo, Huajun Guo, Xinhai Li, Guochun Yan, Qihou Li, Xianglin Li, Ding Wang, Jiexi Wang
    Chinese Chemical Letters. 2024, 35(5): 108638-.

    Ultra-high nickel material is considered to be a promising cathode material. However, with the increase of nickel content, the interfacial side reactions between the cathode and electrolyte become increasingly serious. Herein, an atomically controllable ionic conductor Li3PO4 (LPO) coating is deposited on the LiNi0.90Co0.06Mn0.04O2 (NCM9064) based electrode by the atomic layer deposition method. The results shows that the LPO coating is uniformly and densely covered on the surface of secondary particles of NCM9064, helping to prevent the direct contact between the electrolyte and cathode during the charging-discharging process. In addition, the coating layer is electrochemically stable. As a result, the interfacial side reactions during the long cycle are effectively suppressed, and the solid electrolyte interphase layer at the interface is stabilized. The electrode with 20 layers of LPO deposition (ALD-LPO-20) exhibits an excellent capacity retention of 81% after 200 cycles in 2.8-4.3 V at 25 ℃, which is 18% higher than the unmodified material (ALD-LPO-0). Besides, the moderate LPO coating improves the rate capability and high temperature cycling performance of NCM9064. This study provides a method for the modification of ultra-high nickel cathode materials and corresponding electrodes.

  • Ling Yang, Min Ren, Jie Wang, Liming He, Shanshan Wu, Shuai Yang, Wei Zhao, Hao Cheng, Xiaoming Zhou, Maling Gou
    Chinese Chemical Letters. 2024, 35(5): 108822-.

    Staphylococcal enterotoxin A (SEA) derived from Staphylococcus aureus, as a superantigen, shows potential for cancer immunotherapy, but systemic immunotoxicity restricts its clinical application. Targeted delivery of SEA to tumor site provides a promising option for reducing the systemic toxicity. Here, we constructed an iRGD peptide (H-[Cys-Arg-Gly-Asp-Lys-Gly-Pro-Asp-Cys]-NH2) modified nanoparticle (iDPP) to deliver plasmids encoding SEA for melanoma treatment. The iDPP/SEA nanocomplexes efficiently mediated SEA expression in B16-F10 cells in vivo and in vitro and induced the activation of lymphocytes and maturation of murine bone marrow-derived dendritic cells (BMDCs) in vitro. In the subcutaneous B16-F10 melanoma model, the iDPP/SEA nanocomplexes could effectively enhance immune response and T lymphocytes infiltration in tumor site after intravenous administration, thereby considerably decreased melanoma growth. Meanwhile, no obvious adverse effect was observed after intravenous administration of the iDPP/SEA nanocomplexes in vivo. Our findings demonstrated that gene therapy of SEA is a potential candidate for melanoma treatment.

  • Yihao Zhang, Yang Jiao, Xianchao Jia, Qiaojia Guo, Chunying Duan
    Chinese Chemical Letters. 2024, 35(5): 108748-.

    Porphyrins and their derivatives are excellent photosensitizers in photodynamic therapy (PDT). The modification of porphyrin molecules into metal-organic cages (MOCs) is a viable strategy to improve their bioavailability. In this work, MOC C66 based on porphyrin was synthesised by a one-pot self-assembly method. The three-dimensional structure of the metal-organic cage ameliorated the aggregation and self-quenching of porphyrins and increased the molar absorption coefficient in the visible light region, which enhanced the reactive oxygen species (ROS) yield of porphyrins and effectively improved the efficiency of photodynamic therapy. ROS generation ability tests in solution confirmed the improved reactive oxygen capacity of the cage, which showed greater phototoxicity to HeLa and MCF-7 cells in vitro, suggesting a new strategy for future modifications of the simple synthesis of porphyrins as photosensitizers.

  • Xiaoyao Ma, Jinling Zhang, Ge Fang, He Gao, Jie Gao, Li Fu, Yuanyuan Hou, Gang Bai
    Chinese Chemical Letters. 2024, 35(5): 108823-.

    The clinical benefit of combination therapy is significant, but it is not easy to define the mechanism of complexity and diversity. Previous studies illustrate that phillygenin (Phi) binds in the allosteric inhibit pocket of protein kinase B (AKT), and swertiamarin (Swe) acts on the pleckstrin homology (PH) domain of AKT. However, the combined synergistic effect of relieving the inflammatory response has yet to be elucidated. Based on high sensitivity, specificity and fast-responsibility fluorescent sensors, the Förster resonance energy transfer (FRET) technique offers a route to provide clear insights into physiological and pathological processes. In the study, molecular docking, the fluorescent probes of Phi and Swe for FRET were designed and synthesized. FRET analysis shown that Swe and Phi concurrently acted on the PH domain and allosterically inhibited pocket of AKT, respectively. The combination of Swe and Phi significantly increased the heat stability of AKT and decreased protease-induced degeneration. In lipopolysaccharides (LPS)-induced mice and cells, the combination arrested AKT activation, nuclear factor kappa-B (NF-κB) phosphorylation, and the expression of tumor necrosis factor-α (TNF-α), interleukin (IL)-6 and IL-8. In conclusion, FRET revealed Phi and Swe concurrently targeted AKT on different domains and the combination of Phi and Swe enhanced the anti-inflammatory effect.

  • Tianbo Jia, Lili Wang, Zhouhao Zhu, Baikang Zhu, Yingtang Zhou, Guoxing Zhu, Mingshan Zhu, Hengcong Tao
    Chinese Chemical Letters. 2024, 35(5): 108692-.

    Conversion of CO2 into high-value products using electrochemical CO2 reduction (ECR) technology is an effective way to alleviate global warming and reach carbon neutrality. The oxygen vacancies in heterogenous catalysis are generally considered as a powerful method to enhance the performance of ECR by promoting CO2 adsorption and activation. However, the extent of defects in oxygen vacancies-activity relation has rarely been studied. Herein, we prepared Cu–Cd bimetallic catalysts with adjustable oxygen defect degree by controlling the amount of cadmium addition. Fourier transform infrared spectroscopy characterization results reveal that the formation of oxygen vacancies is attributed to the asymmetric stretching of Cu–O by the addition of cadmium. Electrochemical results show that the oxygen defect degree can modulate the selectivity of ECR products. A low degree of oxygen defects (CuO) is generally associated with lower product Faraday efficiency (FEC2/FEC1 ≈ 114%), but overabundant oxygen vacancies (CuO2.625–CdO0.375) are not entirely favorable to improving ECR activity (FEC2/FEC1 ≈ 125%) and single selectivity, while an appropriate degree of oxygen vacancies (CuO2.75–CdO0.25) can facilitate the ECR process toward single product selective production (FEC2/FEC1 ≈ 296%). The theoretical calculation showed that the O vacancy formed on CuO and the interface between CdO and CuO were conducive to enhancing the formation of *COOH intermediate and promoting the generation of ethylene products. This study provides a new approach and insight into the selective production of single products for future industrial applications of ECR.

  • Hang Chen, Chengzhi Cui, Hebo Ye, Hanxun Zou, Lei You
    Chinese Chemical Letters. 2024, 35(5): 109145-.

    Imine bonds are among the most explored building motifs in dynamic chemistry, polymers, and materials, and yet, their acid-resistance remains a longstanding issue. Herein we demonstrate a concept of internal protecting groups for improving the kinetic stability of dynamic imine bonds and polymers. Systematic examination of structure-reactivity relationship of a series of aldehydes/imines bearing a neighboring carboxyl allowed uncovering of required structural features for dynamically masking imine bonds with cyclic structures. Mechanistic studies indicated that noncovalent interactions along with sterics control the ring-chain equilibrium and the stability of imine bonds. The incorporation of internal protecting groups into imine polymers further enabled their controlled stability in acidic media. Moreover, a combination of dynamic covalent network and coordination supramolecular network provided a facile means for the modulation of luminescent and mechanical properties of polymers. The strategies and results reported should be beneficial to molecular assemblies, dynamic polymers, biological delivery, and intelligent materials.

  • Zixuan Zhu, Xianjin Shi, Yongfang Rao, Yu Huang
    Chinese Chemical Letters. 2024, 35(5): 108954-.

    Integrated CO2 capture and conversion of (ICCC) is one of the most effective solutions to reduce anthropogenic CO2 emissions, which has attracted extensive public attention. Dual functional materials (DFMs), including adsorbent and catalyst, are the key components to achieve ICCC. Magnesium oxide (MgO) is an ideal adsorbent for ICCC, since it is characterized by high theoretical adsorption capacity, low cost, low energy consumption and extensive sources. It can also be used as DFMs in combination with the Ni catalysts. MgO not only can act as an adsorbent in DFMs but also enhance the catalytic performance of Ni. This review summarizes the advantages and modification methods of MgO as adsorbent and the influence of its adsorption conditions on the adsorption performance. Moreover, the important role of MgO in facilitating the catalytic conversion of CO2 is highlighted. Future research focuses are proposed for the development of MgO based DFMs with high adsorption capacity, high stability, conversion, and selectivity as well as low cost and energy consumption.

  • Jianye Kang, Xinyu Yang, Xuhao Yang, Jiahui Sun, Yuhang Liu, Shutao Wang, Wenlong Song
    Chinese Chemical Letters. 2024, 35(5): 109297-.

    Due to the various pH liquid environment in nature, the pH-responsive lubricating hydrogel is widely investigated and developed for tissue interface substitute. However, the applied liquid environment will lead to poor mechanical property and weaken the pH-responsive capability. In this work, a carbon dots-enhanced pH-responsive lubricating hydrogel is developed by combining a pH-responsive section of dynamic PVA-borax network into a PAAm covalent polymer network. The formed hydrogel presents a partial gel-sol transition under controlled pH environments. At low pH environments (< 6.0), the formed lubricating layer originated from dynamic disassembly of PVA-borax hydrogel, and brings the lubricating properties on the hydrogel surface. Moreover, the mechanical strength and lubrication properties are well promoted by introducing the carbon dots into the hydrogel, the blue sol layer can be observed more visually under the fluorescence microscope. The pH-response also exhibits well reversibility. The prepared hydrogel broadens the idea for designing pH-responsive soft materials for soft lubricating actuator or robot.

  • Xinqiong Li, Guocheng Rao, Xi Peng, Chan Yang, Yanjing Zhang, Yan Tian, Xianghui Fu, Jia Geng
    Chinese Chemical Letters. 2024, 35(5): 109419-.

    Diagnostic C9orf72 hexanucleotide repeat expansions (C9-HRE) is essential for the early and accurate diagnosis of amyotrophic lateral sclerosis (ALS) and will provide support for the prognosis and gene therapy of ALS. In the present study, by combining catalytic hairpin assembly (CHA) with Mycobacterium smegmatis porin A (MspA) nanopore, a new nanopore-based strategy for the detection of C9-HRE was reported. Less than 30 repeats of C9-HRE could be detected via this method, and the results have the potential to help distinguish between patients and healthy individuals. Moreover, the method demonstrated its great specificity for C9-HRE by identifying other repeat expansions. Given the high selectivity, this approach had been successfully used to detect C9-HRE in cell and blood samples with high accuracy. This detection strategy is user-friendly and has a strong anti-interference ability, thus providing a powerful tool for clinical diagnosis.

  • Weiwei He, Hongbo Zhang, Xudong Lin, Lili Zhu, Tingting Zheng, Hao Pei, Yang Tian, Min Zhang, Guoyue Shi, Lei Wu, Jianlong Zhao, Gulinuer Wumaier, Shengqing Li, Yufang Xu, Honglin Li, Xuhong Qian
    Chinese Chemical Letters. 2024, 35(5): 109091-.

    This review explores the concept of life-on-a-chip, which involves the creation of miniaturized biological systems, such as organs, tissues, and model organisms, on microscale platforms called microfluidic chips. These chips consist of intricately etched channels, wells, and chambers that enable precise control and observation of fluids, cells, and biochemical reactions, facilitating the simulation of various aspects of human or animal physiology and the study of responses to different stimuli, drugs, or disease conditions. The review highlights the application of a novel technology, "Beyond Limit Manufacturing" (BLM), in the development of sophisticated three-dimensional cell models and model organism microchips. Model-organism-on-a-chip and organ-on-a-chip (OoC) are among the thriving developments in the field of microfluidics, allowing for the reconstruction of living microenvironments and implementation of multiple stimuli. The review discusses the latest advancements in life-on-a-chip technology using BLM and outlines potential future research directions, emphasizing the significant role of these chips in studying complex biological processes in a controlled and scalable manner.

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