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  • Dengqi Xue, Yani Liu, Yilin Zheng, Heling Niu, Liying Dong, Xiangshuo Ouyang, Siyu Song, Denggao Zhang, Qianwei Ge, Kewei Wang, Liming Shao
    Chinese Chemical Letters. 2022, 33(3): 1643-1646.

    Three novel series of α-aminoamides derivatives were designed and synthesized based on ralfinamide, and their Nav1.7 inhibitory activities were evaluated using manual patch clamp electrophysiology. Active compounds inhibited Nav1.7 with half maximal inhibitory concentration (IC50) values ranging from 2.9 µmol/L to 21.4 µmol/L. Among them, the most potent compound 19h exhibited about 12-fold potency better than ralfinamide. The investigation of their structure-activity relationship gives a strategy to improve the Nav1.7 inhibition of ralfinamide analogues. Compound 19h was efficacious in antinociception in the mouse spared nerve injury (SNI) model of neuropathic pain without causing sedation in the open field test.

  • Zhiwei Wang, Qishun Liu, Ruisheng Liu, Zhongyin Ji, Yan Li, Xiaohui Zhao, Wei Wei
    Chinese Chemical Letters. 2022, 33(3): 1479-1482.

    A mild and efficient photochemical multi-component tandem reaction of quinoxalin-2(1H)-ones, alkenes and sulfinic acids is reported. This tandem reaction could be conveniently carried out at room temperature by employing 4CzIPN as the metal-free photocatalyst and dioxygen (air) as the environmentally benign oxidant. A number of sulfonated quinoxalin-2(1H)-ones were obtained in satisfactory yields with favorable functional group tolerance. Radical trapping experiment and fluorescence quenching experiments were performed to elucidate this visible-light mediated radical reaction process.

  • Jing Chen, Yumei Tang, Shihao Wang, Lingbin Xie, Cheng Chang, Xiaolei Cheng, Mingming Liu, Longlu Wang, Lianhui Wang
    Chinese Chemical Letters. 2022, 33(3): 1468-1474.

    Molybdenum disulfide (MoS2) with low cost, high activity and high earth abundance has been found to be a promising catalyst for the hydrogen evolution reaction (HER), but its catalytic activity is considerably limited due to its inert basal planes. Here, through the combination of theory and experiment, we propose that doping Ni in MoS2 as catalyst can make it have excellent catalytic activity in different reaction systems. In the EY/TEOA system, the maximum hydrogen production rate of EY/Ni-Mo-S is 2.72 times higher than that of pure EY, which confirms the strong hydrogen evolution activity of Ni-Mo-S nanosheets as catalysts. In the lactic acid and Na2S/Na2SO3 systems, when Ni-Mo-S is used as co-catalyst to compound with ZnIn2S4 (termed as Ni-Mo-S/ZnIn2S4), the maximum hydrogen evolution rates in the two systems are 5.28 and 2.33 times higher than those of pure ZnIn2S4, respectively. The difference in HER enhancement is because different systems lead to different sources of protons, thus affecting hydrogen evolution activity. Theoretically, we further demonstrate that the Ni-Mo-S nanosheets have a narrower band gap than MoS2, which is conducive to the rapid transfer of charge carriers and thus result in multi-photocatalytic reaction systems with excellent activity. The proposed atomic doping strategy provides a simple and promising approach for the design of photocatalysts with high activity and stability in multi-reaction systems.

  • Li-Jun Xie, Cui-Lian Lin, Li Liu, Liang Cheng
    Chinese Chemical Letters. 2022, 33(3): 1563-1566.

    N6-methyl adenosine (m6A) is an eminent epigenetic mark in mRNAs that affects a broad range of biological functions in diverse species. However, the chemically inert methyl group prevents a direct labeling of this modification for subsequent detection and sequencing. Therefore, most current approaches for the labeling of m6A still have limitations of relying on the utilization of corresponding methyltransferases, which resulted in the lacking of efficiency. Here we present an approach which selectively alkylated the N6-formyl adenosine (f6A), the key intermediate during chemical oxidation of m6A, with an alkyne functionality that can be further labeled with click reactions. This covalent labeling approach will be able to facilitate in the affinity purification, detection and genome-wide profiling studies.

  • Yuxuan Wang, Qifeng Zhou, Xiaoxiao He, Ying Zhang, Hongwei Tan, Jianhua Xu, Cuihong Wang, Wei Wang, Xiping Luo, Jinquan Chen, Lin Xu
    Chinese Chemical Letters. 2022, 33(3): 1613-1618.

    It has been challenging to achieve multi-photochromic systems without affecting the individual photoswitching properties of the constituent units. Herein, we present the design and synthesis of a new family of platinum-acetylide dendrimers containing up to twenty-one photochromic dithienylethene (DTE) units that exhibit both high photochromic efficiency and individual switching properties. Upon irradiation with ultraviolet (UV) and visible (vis) light, the resultant metallodendrimers display high conversion yield and good fatigue resistance. More interestingly, cyclization-cycloreversion kinetics revealed that the photochromic property of each DTE unit in these metallodendrimers is unaffected by its neighbor and the full ring-closure of up to twenty-one DTE units in one single dendrimer has been achieved.

  • Jian-Jun Dai, Xin-Xin Teng, Wen Fang, Jun Xu, Hua-Jian Xu
    Chinese Chemical Letters. 2022, 33(3): 1555-1558.

    An electrochemically promoted decarboxylative borylation reaction is reported. The reaction proceeds under mild conditions in an undivided cell without use of transition metal- or photo-catalysts. The key feature of the reaction is the compatibility of diboron reagents with the electrochemical conditions. This reaction exhibits broad substrate scope, good functional group tolerability, and easy scalability.

  • Siyang Jiang, Weipeng Mao, Dake Mao, Zhan-Ting Li, Da Ma
    Chinese Chemical Letters. 2022, 33(2): 881-884.

    We report supramolecular AND logic gates based on host-guest complexation between acid-labile acyclic cucurbit[n]uril (CB[n]) molecular container and NaClO-responsive dye. Supramolecular AND logic gate is turned on due to acid-triggered degradation of molecular container and the release of the dye, followed by NaClO-induced fluorescence "switch on" effect of the dye. The reason for AND molecular logic gate is discovered to be the combination of oxidation inhibition and fluorescence "switch off" effect. Supramolecular AND logic gate is confirmed to be operational in live MCF-7 and HeLa cancer cells.

  • De-Ao Xu, Qing-Yang Zhou, Xianyin Dai, Xin-Kun Ma, Ying-Ming Zhang, Xiufang Xu, Yu Liu
    Chinese Chemical Letters. 2022, 33(2): 851-854.

    A phosphorescent supramolecular foldamer is conveniently constructed by the 1:1 host–guest complexation with cucurbit[8]uril and 1, 2-diaminocyclohexane-bridged 4-(4-bromophenyl)-pyridinium salt. The tightly compact host–guest complexation in molecular foldamer can greatly suppress the fluorescence emissive channel and promote the intersystem crossing from singlet to triplet states, thus leading to the green phosphorescence at ambient temperature in aqueous solution. More intriguingly, the phosphorescence emission shows very rapid and sensitive responsiveness to different antibiotics in both inanimate milieu and living cells. Remarkably, the limit of detection of such binary inclusion complex toward sulfamethazine can reach as low as 1.86 × 10−7 mol/L. Thus, it is envisaged that this supramolecular nanoplatform featuring unique complexation-enhanced phosphorescence emission may hold great promise in sensing and detecting many other biological targets under physiological environment.

  • Xiaohan Cao, Hongliang Wang, Jialiang Yang, Ruiyang Wang, Xin Hong, Xinghong Zhang, Junting Xu, Hai Wang
    Chinese Chemical Letters. 2022, 33(2): 1021-1024.

    In this paper, the crystallization behavior of a novel poly(monothiocarbonate), poly(trimethylene monothiocarbonate) (PTMMTC), was investigated and compared with its polycarbonate analogue, poly(trimethylene carbonate) (PTMC). It is found that PTMMTC exhibits strong crystallizability, while unstretched PTMC is amorphous. DSC and DMA results reveal that PTMMTC possesses higher glass transition temperature (Tg) and β-transition temperature (Tβ) than PTMC. Simulation based on density functional theory (DFT) shows that, the bond angle of C-S-C is evidently smaller than that of C-O-C, and thus a larger dipole moment. This leads to the stronger intermolecular interaction and more rigid chain conformation in PTMMTC, which is the origin of sulfur-substitution enhanced crystallization. The crystal structure of PTMMTC was preliminarily determined for the first time. PTMMTC has an orthorhombic crystal structure with a planar zig-zag chain conformation. The parameters of unit cell are a = 10.74 Å, b = 4.79 Å, and c (fiber axis) = 7.74 Å.

  • Zhen Chen, Ce Bian, Chi Fan, Tao Li
    Chinese Chemical Letters. 2022, 33(2): 893-897.

    Si coordination structures have been proven to greatly influence the ammonia-selective catalytic reduction (NH3-SCR) catalytic properties and the hydrothermal stability of Cu-based silicoaluminophosphate-form catalysts. However, the role of various Si coordination structures in the NH3-SCR reaction over Cu-SAPO-34 catalyst remains unknown. Herein, a batch of Cu-SAPO-34 samples with various Si contents was synthesized via a one-pot method to study the role of Si coordination structures in the NH3-SCR catalytic properties and hydrothermal stability. Cu/34–2 with the highest proportion of Si(xOAl) (x = 1~3) structures exhibits remarkable durability with 90% NO reduction efficiency within 200~450 ℃ even after a hydrothermal aging treatment at 850 ℃. In contrast, Cu/34–1 and Cu/34–4 with the highest proportions of Si(4OAl) and Si(0OAl) structures, respectively, are significantly deactivated by the same hydrothermal treatment. To better understand this phenomenon, the relationship between the Si coordination structures and SCR performance is established using characterization techniques and kinetics measurements. Results reveal that a high content of Si(4OAl) and Si(0OAl) is detrimental to the hydrothermal stability of Cu-SAPO-34 catalyst. However, Si(xOAl) (x = 1~3) structures are conducive to the stabilization of isolated Cu2+, thus enhancing the stability to severe hydrothermal treatment.

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