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  • Muzi Li, Wen Zhang, Jiaxin Li, Yinghe Qi, Chen Peng, Nan Wang, Huili Fan, Yan Li
    Chinese Chemical Letters. 2023, 34(11): 108177-.

    Nanocarriers play an important role in drug delivery for disease treatment. However, nanocarriers face a series of physiological barriers after administration such as blood clearance, nonspecific tissue/cell localization, poor cellular uptake, and endosome trapping. These physiological barriers seriously reduce the accumulation of drugs in target action site, which results in poor therapeutic efficiency. Although polyethylene glycol (PEG) can increase the blood circulation time of nanocarriers, its application is limited due to the "PEG dilemma". Zwitterionic polymers have been emerging as an appealing alternative to PEG owing to their excellent performance in resisting nonspecific protein adsorption. Importantly, the diverse structures bring functional versatility to zwitterionic polymers beyond nonfouling. This review focuses on the structures and characters of zwitterionic polymers, and will discuss and summarize the application of zwitterionic polymers for drug delivery. We will highlight the strategies of zwitterionic polymers to address the physiological barriers during drug delivery. Finally, we will give some suggestions that can be utilized for the development of zwitterionic polymers for drug delivery. This review will also provide an outlook for this field. Our aim is to provide a comprehensive and systemic review on the application of zwitterionic polymers for drug delivery and promote the development of zwitterionic polymers.

  • Yunying Xu, Aiyou Hao, Pengyao Xing
    Chinese Chemical Letters. 2023, 34(11): 108492-.

    Distortion of planar aromatics occurs in the fused rings conjugated with bulky substituents, which generates racemic enantiomers with high transformation energy barriers. However, direct synthesis of homochiral distorted aryl compounds is a very challenging task. Here, we presented a molecular folding strategy to control distorted aryl homochirality. Amino acids and their derivatives conjugated on the polycyclic aromatic hydrocarbons including benzenes, naphthalenes and triphenylenes, which formed parallel β-sheet arrays through intramolecular hydrogen bonds. The folding behavior enabled distorted or twisted geometry of aromatics, of which the handedness was associated with the absolute chirality of amino acids. X-ray crystallography, theoretical calculations and circular dichroism spectroscopy verified the distorted homochirality in the solid and solution phase. The relatively small rotational barrier between the enantiomers made the molecule sensitive to the environment and thus realized the solvent-controlled chiral inversion. The β-sheet folding strategy can be widely used in polycyclic aromatic hydrocarbons with various functions, which provided a promising strategy to control inherent chirality of aromatics with adaptive chiroptical responses.

  • Shihao Chen, Zhishang Zhang, Li Wei, Zhongxian Fan, Yue Li, Xuezhi Wang, Tongming Feng, Huaiyi Huang
    Chinese Chemical Letters. 2023, 34(11): 108412-.

    Bacterial infection is currently a serious challenge globally, causing death of thousands of human beings. New antimicrobial agents with novel mechanism of action are urgently needed. Transition metal complexes have shown great potentials in photodynamic and photocatalytic therapy. Herein, we take full advantage of metal photocatalyst and successfully developed a novel cyclometalated iridium(Ⅲ) complex (Ir1) with higher biofilm damage efficiency than the clinical antibiotics. Ir1 synergistically generates reactive oxygen species and coenzyme photocatalytic activity with high efficiency under white light irradiation. Combined with these properties, Ir1 exhibited excellent photoinactivation of S. aureus and effectively damaged the biofilm. This work provides a new approach for the development of antibacterial photodynamic therapy.

  • Haochang Zhang, Zhaozhe Yu, Jinyin Cheng, Hannan Chen, Xiao Huang, Bingbing Tian
    Chinese Chemical Letters. 2023, 34(11): 108228-.

    Li2ZrCl6 (LZC) solid-state electrolytes (SSEs) have been recognized as a candidate halide SSEs for all-solid-state Li batteries (ASSLBs) with high energy density and safety due to its great compatibility with 4 V-class cathodes and low bill-of-material (BOM) cost. However, despite the benefits, the poor chemical/electrochemical stability of LZC against Li metal causes the deterioration of Li/LZC interface, which has a detrimental inhibition on Li+ transport in ASSLBs. Herein, we report a composite SSE combining by LZC and argyrodite buffer layer (Li6PS5Cl, LPSC) that prevent the unfavorable interaction between LZC and Li metal. The Li/LPSC-LZC-LPSC/Li symmetric cell stably cycles for over 1000 h at 0.3 mA/cm2 (0.15 mAh/cm2) and has a high critical current density (CCD) value of 2.1 mA/cm2 at 25 ℃. Under high temperature (60 ℃) which promotes the reaction between Li and LZC, symmetric cell fabricated with composite SSE also display stable cycling performance over 1200 h at 0.3 mAh/cm2. Especially, the Li/NCM ASSLBs fabricated with composite SSE exhibit a high initial coulombic efficiency, as well as superior cycling and rate performance. This simple and efficient strategy will be instrumental in the development of halide-based high-performance ASSLBs.

  • Xiaoyu Shao, Shujing Xu, Xufeng Wan, Yang Zhou, Shuo Wang, Shuo Wu, Yuhuan Li, Xinyong Liu, Peng Zhan
    Chinese Chemical Letters. 2023, 34(11): 108349-.

    Despite the improving coverage of preventative vaccines,hepatitis B remains a severe global public health problem,with more than 250 million patients living with hepatitis B virus (HBV) infection. Current available therapies,including nucleos(t)ide analogs and peginterferon,can control HBV replication but fail to eliminate covalently closed circular DNA (cccDNA) and achieve a cure. The HBV core protein (Cp) is a well-conserved structural protein,self-assembling to form the viral capsid. It involves in or modulates almost every stage of the HBV lifecycle,which makes it an attractive target for the development of new anti-HBV therapies. HBV core protein allosteric modulators (CpAMs) have become a hotspot in recent years. Herein,we provide a concise report focusing on the various medicinal chemistry strategies involved in the latest research (2018–2022) of HBV CpAMs,including high throughput screening (HTS),virtual screening (VS),drug repositioning,natural products,substitution decorating approach,scaffold hopping,molecular hybridization,prodrug strategy and conformational constraint strategy,to provide guidance for further development of new and effective anti-HBV drugs.

  • Yuwei Zhao, Chang Liu, Chenyang Zha, Jing Li, Chongguang Lyu, Kaixi Wang, Junfeng Li, Kwan San Hui, Linghai Zhang, Kwun Nam Hui
    Chinese Chemical Letters. 2023, 34(11): 108189-.

    The d-band centers of catalysts have exhibited excellent performance in various reactions. Among them, the enhanced catalytic reaction is considered a crucial way to power dynamics and reduce the "shuttle" effect in polysulfide conversions of lithium-sulfur batteries. Here, we report two-dimensional-shaped tungsten borides (WB) nanosheets with d-band centers, where the d orbits of W atoms on the (001) facets show greatly promoting the electrocatalytic sulfur reduction reaction. As-prepared WB-based Li-S cells exhibit excellent electrochemical performance for Li-ion storage. Especially, it delivers superior capacities of 7.7 mAh/cm2 under the 8.0 mg/cm2 sulfur loading, which is far superior to most other electrode catalysts. This study provides insights into the d-band centers as a promising catalyst of two-dimensional boride materials

  • Gamal H. Al-Shawesh, Jiawen Zhu, Wei Zhang, Shuai Xie, Junjie Xu, Guolei Cai, Amar Y. Al-Ansi, Yunhong Wei, Song Jin, Hengxing Ji
    Chinese Chemical Letters. 2023, 34(11): 108190-.

    The undesirable shuttle effect and sluggish redox kinetics of polysulfides seriously result in low sulfur utilization and poor capacity retention. Here, an integrated strategy is proposed by rational designing multifunctional architecture to manipulate the redox kinetics of polysulfides, specifically, by employing iron atoms (Fe-As) and iron-species nanoparticles (Fe-NPs) co-embedded nitrogen-doped carbon nanotube (Fe-NCNT) as catalyst and host for sulfur. The synergistic cooperation of Fe-As and Fe-NPs provides efficient active sites to facilitate the diffusion, strengthen the affinities, and promote the conversion reactions for polysulfides. Furthermore, the NCNT not only offers practical Li+ transport pathways but also immobilize the polysulfides effectively. Benefiting from these merits, the Fe-NCNT/S electrodes exhibit high initial specific capacity of 1502.6 mAh/g at 0.1 C, outstanding rate performance (830 mAh/g at 2 C), and good cycling performance (597.8 mAh/g after 500 cycles with an ultralow capacity fading rate of 0.069% per cycle). This work features the distinct interaction of iron atom-nanoparticles on facilitating immobilization-diffusion-transformation process of polysulfides, and it also expected to pave the way for the application in practical Li-S batteries.

  • Taoyuan Xiu, Simei Zhang, Peng Ren, Siyan Liu, Shuai Wang, Hamza Shehzad, Jingyang Wang, Meng Zhang, Guoan Ye, Caishan Jiao, Qunyan Wu, Liyong Yuan, Zhifang Chai, Weiqun Shi
    Chinese Chemical Letters. 2023, 34(11): 108440-.

    Uranium and molybdenum are important strategic elements. The production of 99Mo and the hydrometallurgical process of uranium ore face difficult problems of separation of uranium and molybdenum. In this study, the four phenanthroline diamide ligands were synthesized, and extraction and stripping experiments were performed under different conditions to evaluate the potential application of these ligands for separation of U(Ⅵ) over Mo(Ⅵ). With the growth of alkyl chain, the solubility of ligands could be greatly improved, and the separation effect of U(Ⅵ) over Mo(Ⅵ) gradually increased. The SFU/Mo were around 10,000 at 4 mol/L HNO3. Three stripping agents were tested with the stripping efficiency of Na2CO3 (5%) > H2O > HNO3 (0.01 mol/L). The stripping percentages of the three stripping agents were all close to unity, indicating that the ligands had the potential to be recycled. The chemical stoichiometry of U(Ⅵ) complexes with ligands was evaluated as 1:1 using electrospray ionization mass spectrometry, ultraviolet visible spectroscopy and single-crystal X-ray diffraction. The consistency between theoretical calculation and experimental results further explains the coordination mechanism.

  • Feng Liu, Xin Wang, Meng Wang, Yao Li, Zishuai Jiang, Wenbo Zhang, Haiyue Yang, Chengyu Wang, Shih-Hsin Ho
    Chinese Chemical Letters. 2023, 34(11): 108353-.

    While superhydrophobic coatings have shown promise as potential anti-icing coatings, the surface roughness of these coatings is prone to damage during repeated icing-deicing cycles. Herein, two kinds of superhydrophobic anti-icing coatings are prepared from organic resin and micro-nano particles using two strategies, and their excellent anti-icing properties are also investigated. However, superhydrophobic surface Ⅰ (SF1), prepared by first strategy, cannot be used for extended periods of time due to irreversible damage to the surface roughness during the icing–deicing process. Finite element simulations and experimental studies are preformed to investigate the fatal issue of such roughness damage. In contrast, the anti-icing properties of superhydrophobic surface Ⅱ (SF2), prepared by second strategy, can easily regain through a simple sandpaper abrasion treatment even the surface roughness was damaged during the icing–deicing process. These exploratory results and SF2 preparation strategy provide a facile design of anti-icing coating, and the derived restorable anti-icing coating is expected to be useful for a wide application.

  • Jianjian Yi, Zhou Zhou, Yu Xia, Ganghua Zhou, Guoxiang Zhang, Li Li, Xuyu Wang, Xingwang Zhu, Xiaozhi Wang, Huan Pang
    Chinese Chemical Letters. 2023, 34(11): 108328-.

    In this work, taking NiSe2 as a prototype to be used as cocatalyst in photocatalytic hydrogen evolution, we demonstrate that the crystal phase of NiSe2 plays a vital role in determining the catalytic stability, rather than activity. Theoretical and experimental results indicate that the phase structure shows negligible influence to the charge transport and hydrogen adsorption capacity. When integrating with carbon nitride (CN) photocatalyst forming hybrids (m-NiSe2/CN and p-NiSe2/CN), the hybrids show comparable photocatalytic hydrogen evolution rates (3.26 µmol/h and 3.75 µmol/h). Unlike the comparable catalytic activity, we found that phase-engineered NiSe2 exhibits distinct stability, i.e., m-NiSe2 can evolve H2 steadily, but p-NiSe2 shows a significant decrease in catalytic process (~57.1% decrease in 25 h). The factor leading to different catalytic stability can be ascribed to the different surface conversion behavior during photocatalytic process, i.e., chemical structure of m-NiSe2 can be well preserved in catalytic process, but partial p-NiSe2 tends to be converted to NiOOH.

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