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  • Yan Zou, Yin-Shuang Hu, Deng-Hui Tian, Hong Wu, Xiaoshu Lv, Guangming Jiang, Yu-Xi Huang
    Chinese Chemical Letters. 2024, 35(6): 109090-.

    Membrane-based separation is a promising technology to eliminate water impurities from the oil phase. However, it remains a great challenge to separate water from highly emulsified viscous oil owing to the high stability of the water droplets in oil. Herein we report a surface wettability engineering on an alumina ceramic membrane to achieve an efficient separation of a water-in-oil (W/O) emulsion. Silanes with different carbon chain lengths and fluorinated status were introduced to endow the alumina membrane with different surface wettabilities. While all the modified membranes exhibited excellent separation of the W/O without Span 80 (surfactant), the one with amphiphobic wettability and lowest surface energy failed to separate the Span 80 stabilized W/O. The presence of Span 80 reduced the interfacial tension of water droplets, making them easier to deform and penetrate the modified membrane with the lowest surface energy. It reveals that engineering proper surface wettability is the key to separating the oil and water phases. Besides, the modified membranes maintained decent separation performance and stability under long-term run separation of the emulsified W/O.

  • Tian Yang, Yi Liu, Lina Hua, Yaoyao Chen, Wuqian Guo, Haojie Xu, Xi Zeng, Changhao Gao, Wenjing Li, Junhua Luo, Zhihua Sun
    Chinese Chemical Letters. 2024, 35(6): 108707-.

    Molecular dielectric switches constitute a type of intelligent materials that are highly coveted for their distinctive advantages of switchable dielectric responses, lightweight, and mechanical flexibility. Two-dimensional (2D) hybrid perovskites have demonstrated excellent promise for assembling dielectric switches, in which the dynamic motions of organic moieties afford driving force to trigger switchable dielectric phase transition. Here, we successfully assembled a new lead-free hybrid double perovskite, (CHA)4CuBiBr8 (1, CHA = cyclohexylammonium), adopting a typical 2D structural motif, which shows dielectric anisotropy and bistable behaviors during the reversible phase transition near Tc = 378 K (the Curie temperature). That is, its dielectric constants could be switched and tuned between high-dielectric and low-dielectric states. Structure analyses reveal that the ordered-disordered transformation of the organic CHA+ moiety and distortion of inorganic framework account for its phase transition. This result will stimulate further exploration of molecular dielectric switches in this 2D environmentally friendly family.

  • An Lu, Yuhao Guo, Yi Yan, Lin Zhai, Xiangyu Wang, Weiran Cao, Zijie Li, Zhixia Zhao, Yujie Shi, Yuanjun Zhu, Xiaoyan Liu, Huining He, Zhiyu Wang, Jian-Cheng Wang
    Chinese Chemical Letters. 2024, 35(6): 108928-.

    Immunosuppressive microenvironments present critical problems in clinical chemotherapy. To regulate the tumor immune microenvironment for enhancing antitumor effect, a combination of immune checkpoint inhibitors (ICIs) with chemotherapeutics has been applied clinically. In this study, miriplatin (MiPt), the lipidic derivative of 5-fluorouracil (Fu-OA), as well as the programmed death ligand 1 (PD-L1) target siRNA (siPD-L1) were integrated into Lip-Pt/Fu@siPD-L1 nanoparticles (NPs) for chemo-immunotherapy. In vitro results showed that Lip-Pt/Fu@siPD-L1 NPs could exhibit effective siRNA gene silencing and promote the phagocytosis of tumor cells by macrophages. Furthermore, in vivo results revealed that Lip-Pt/Fu@siPD-L1 NPs showed significantly higher anti-tumor efficiency than that of the physical mixing of MiPt, 5-fluorouracil, and Lip@siPD-L1 NPs (delivery of siPD-L1 by liposomes). The best anti-tumor efficiency of Lip-Pt/Fu@siPD-L1 NPs resulted from the synergistic immunotherapeutic effects of MiPt and siPD-L1 based on the inhibition of CD47 expression and the downregulation of PD-L1 in tumor cells, which elicited a robust anti-tumor immune response through the activation of macrophage phagocytosis and immune checkpoint inhibition. The Lip-Pt/Fu@siPD-L1 NPs provide a potential strategy for tumor chemo-immunotherapy.

  • Hao Deng, Yuxin Hui, Chao Zhang, Qi Zhou, Qiang Li, Hao Du, Derek Hao, Guoxiang Yang, Qi Wang
    Chinese Chemical Letters. 2024, 35(6): 109078-.

    In recent years, the emerging two−dimensional material−MXenes has attracted widespread attention in the field of photocatalysis due to its high conductivity, suitable Fermi level, tunable elemental composition, and excellent photoelectric properties. The zero−dimensional quantum dots (MQDs) derived from 2D MXenes not only inherit the characteristics of MXenes but also exhibit better performance due to the quantum size effect. Based on the above excellent physical and chemical properties, MQDs are often used as co−catalysts of photocatalysts, and show excellent co−catalytic properties. At the same time, compared with other cocatalysts (precious metals, metal oxides, metal sulfides), it has the advantages of low cost and high conductivity. Therefore, understanding the status of MQDs in the field of photocatalysis is crucial for their further development. In this review, we summarized the synthesis and modification methods of MQDs in recent years, as well as their photocatalytic applications in H2 production, CO2 reduction, N2 fixation, pollutant degradation, and other aspects. In addition, the challenges and prospects faced by MQDs are also proposed, providing theoretical guidance for the further development of MQD−based photocatalysts.

  • 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.

  • Jiale Zheng, Mei Chen, Huadong Yuan, Jianmin Luo, Yao Wang, Jianwei Nai, Xinyong Tao, Yujing Liu
    Chinese Chemical Letters. 2024, 35(6): 108812-.

    Lithium (Li) metal anodes (LMAs) have garnered significant attention as a potential solution for developing high-energy density batteries, given their theoretical specific capacity and redox potential. However, safety concerns and internal cycling stability issues originated from uncontrollable Li dendrite growth have impeded the practical application of LMAs. Probing the interface between Li metal and electrolyte is a crucial process that offers valuable insights into the characteristics and regularity of primary circular reactions. To illustrate the intrinsic characteristic of Li metal batteries (LMBs) in spatial and temporal, it is imperative to employ electron microscopes to characterize the structural components distribution of Li with atomic resolution. This paper summarizes the progress in the characterization and analysis of the interfaces in LMBs with electron microscopes based on the principles of electron-matter interactions. Finally, future trends and the potential of electron microscopes are also discussed to advance our understanding of LMBs.

  • Yue Qian, Zhoujia Liu, Haixin Song, Ruize Yin, Hanni Yang, Siyang Li, Weiwei Xiong, Saisai Yuan, Junhao Zhang, Huan Pang
    Chinese Chemical Letters. 2024, 35(6): 108785-.

    Covalent organic frameworks (COFs) exhibiting reversible redox behaviors have been identified as promising candidates for constructing electrode materials in lithium-ion batteries (LIBs). However, their extensive application has been limited due to finite redox sites and poor structural stability. In this study, we design and synthesize a novel polyimide covalent organic framework (PI-COF) using the traditional solvothermal method and successfully apply it as an anode material for LIBs. The large conjugated structure of PI-COF accelerates charge transfer, while its large surface area provides more active sites, making PI-COF an attractive anode material for LIBs. Furthermore, the PI-COF anode material demonstrates high reversible specific capacity and excellent long-term cycling stability due to its COF characteristics. Specifically, the PI-COF electrodes deliver a specific capacity of 800 mAh/g at a current density of 200 mA/g after 200 cycles, while a specific capacity of 450 mAh/g at a current density of 1000 mA/g is sustained after 800 cycles. The outstanding lithium storage capacity, particularly the satisfactory long-term cycling stability, establishes PI-COF as a promising material for LIBs.

  • Chaochao Wei, Ru Wang, Zhongkai Wu, Qiyue Luo, Ziling Jiang, Liang Ming, Jie Yang, Liping Wang, Chuang Yu
    Chinese Chemical Letters. 2024, 35(6): 108717-.

    FeS2 shows significant potential as cathode material for all-solid-state lithium batteries (ASSLBs) due to its high theoretical specific capacity, low cost, and environmental friendliness. However, the poor ion/electron conductivity and large volume variation effect of FeS2 inhibit its practical applications. Here, the influence of particle size of FeS2 on the corresponding sulfide-based solid-state batteries is carefully investigated by tuning FeS2 size. Moreover, low operating temperature is chosen to mitigate the large volume changes during cycling in the battery. S-FeS2 with smaller particle sizes delivers superior electrochemical performances than that of the larger L-FeS2 in Li5.5PS4.5Cl1.5-based ASSLBs under different operating temperatures. S-FeS2 shows stable discharge capacities during 50 cycles with a current density of 0.1 mA/cm2 under -20 ℃. When the current density rises to 1.0 mA/cm2, it delivers an initial discharge capacity of 146.9 mAh/g and maintains 63% of the capacity after 100 cycles. This work contributes to constructing ASSLBs enables excellent electrochemical performances under extreme operating temperatures.

  • 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.

  • Long Li, Kang Yang, Chenpeng Xi, Mengchao Li, Borong Li, Gui Xu, Yuanbin Xiao, Xiancai Cui, Zhiliang Liu, Lingyun Li, Yan Yu, Chengkai Yang
    Chinese Chemical Letters. 2024, 35(6): 108814-.

    Side reactions and dendrite growth triggered by the unstable interface and inhomogeneous deposition have become the biggest obstacle to the commercialization for lithium metal batteries. In this study, a highly-chlorinated organic-inorganic hybrid interfacial protective layer is developed by rationally tuning the interfacial passivation and robustness to achieve the convenient and efficient Li metal anode. The polyvinyl chloride (PVC) can effectively resist water and oxygen, which is confirmed by density functional theory. The organic-dominant solid electrolyte interphases (SEI) with lithium chloride are investigated by the X-ray photoelectron spectroscopy (XPS) with little mineralization of oxide, such as Li2O and Li2CO3. With such artificial SEI, a uniform and dense lithium deposition morphology are formed and an ultra-long stable cycle of over 500 h are achieved even at an ultra-high current density of 10 mA/cm2. Moreover, the simple and convenient protected anode also exhibits excellent battery stability when paired with the LiNi0.8Co0.1Mn0.1O2 (NCM811) and LiFePO4 (LFP) cathode, showing great potential for the commercial application of lithium metal batteries.

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