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  • Zhen Zhang, Fang Chen, Jiwen Feng, Junfei Chen, Li Chen, Zhi Zhang, Huijuan Wang, Xin Cheng, Maili Liu, Chaoyang Liu
    Chinese Chemical Letters. 2021, 32(11): 3483-3486.

    Nanodiamond (ND) polarizer can be used for dynamic nuclear polarization (DNP), owing to unpaired electrons provided by surface defects. However, 1H enhancement via Overhauser DNP (ODNP) using ND in-situ liquid has been found much smaller than traditional radicals. Herein, we study the surface properties of ND using electron spin resonance (ESR) and Raman methods firstly. Then the enhancement of 1H ODNP is explored using ND as polarizer with different nanoparticle sizes and concentrations at home-built 0.06 T DNP spectrometer. The surface of ND with the size of 30 nm is further modification via high temperature air oxidized and the enhancement was measured. The results show that nanoparticle sizes and Raman peak intensity ratio of sp2/sp3 hybridization are approximate negative correlation and positive correlation to enhancement, respectively. Furthermore, there is no significant enhancement in the oxidation group, and a −22.5-fold 1H ODNP enhancement is achieved in-situ liquid at room temperature, which demonstrate the ND can be used as an efficient enhancer. We expect ND to play a greater role in biomedical research, especially for multimodal imaging with improving the performance of ND surface.

  • Yuqi Chen, Mengna Jiang, Liwei Xiong, Xianxian Yao, Mingjian Fan, Danyang Chen, Qi Jiang, Zhaokui Jin, Qianjun He
    Chinese Chemical Letters. 2021, 32(11): 3487-3490.

    The development of multifunctional theranostic nano-agents is an important resolution for personalized treatment of cancer. In this work, we synthesized a new kind of gadolinium boride nanoparticles (GBN) by a microwave-assisted chemical etching method, and discovered their optical characteristics including fluorescence imaging and near-infrared (NIR) photothermal conversion capability. Bright greenishyellow fluorescence enabled for intracellular localization, while effective NIR-photothermal conversion supported photothermal therapy (PTT). In vitro and in vivo results indicated that GBN exhibited a superior antitumor performance and high biocompatibility. This study demonstrated a promising multifunctional theranostic nanoplatform for cancer treatment.

  • Xueli Guo, Liang Xiao, Pengfei Yan, Ming Li, Mingjun Zhu, Jinping Liu
    Chinese Chemical Letters. 2021, 32(11): 3491-3495.

    Modifying electrochemical surface area (ECSA) and surface chemistry are promising approaches to enhance the capacities of oxygen cathodes for lithium-oxygen (Li-O2) batteries. Although various chemical approaches have been successfully used to tune the cathode surface, versatile physical techniques including plasma etching etc. could be more effortless and effective than arduous chemical treatments. Herein, for the first time, we propose a facile oxygen plasma treatment to simultaneously etch and modify the surface of Co3O4 nanosheet arrays (NAs) cathode for Li-O2 batteries. The oxygen plasma not only etches Co3O4 nanosheets to enhance the ECSA but also lowers the oxygen vacancy concentration to enable a Co3+-rich surface. In addition, the NA architecture enables the full exposure of oxygen vacancies and surface Co3+ that function as the catalytically active sites. Thus, the synergistic effects of enhanced ECSA, modest oxygen vacancy and high surface Co3+ achieve a significantly enhanced reversible capacity of 3.45 mAh/cm2 for Co3O4 NAs. This work not only develops a promising high-capacity cathode for Li-O2 batteries, but also provides a facile physical method to simultaneously tune the nanostructure and surface chemistry of energy storage materials.

  • Qizhi Zhong, Bao Liu, Bingjun Yang, Yali Li, Junshuai Li, Xingbin Yan
    Chinese Chemical Letters. 2021, 32(11): 3496-3500.

    The rapid development of next-generation flexible electronics stimulates the growing demand for flexible and wearable power sources with high energy density. Li metal capacitor (LMC), combining with a Li metal anode and an activated carbon cathode, exhibits extremely high energy density and high power density due to the unique energy storage mechanism, thus showing great potential for powering wearable electronic devices. Herein, a flexible LMC based on an in situ prepared PETEA-based gel polymer electrolyte (GPE) was reported for the first time. Owing to the high ionic conductivity of PETEA-based GPE (5.75 × 10-3 S/cm at 20 ℃), the assembled flexible LMC delivers a high capacitance of 210 F/g at 0.1 A/g within the voltage range from 1.5 V to 4.3 V vs. Li/Li+, a high energy density of 474 Wh/kg at 0.1 A/g and a high power density of 29 kW/kg at 10 A/g. More importantly, PETEA-based GPE endows the LMC with excellent flexibility and safety, which could work normally under abuse tests, such as bending, nail penetration and cutting. The in situ prepared PETEA-based GPE simplifies the fabrication process, avoids the risk of leakage and inhibits the growth of Li dendrite, making LMC a promising flexible energy storage device for the flexible electronic field.

  • Pengyuan Qiu, Jianwei Wang, Zhangqian Liang, Yanjun Xue, Yanli Zhou, Xiaoli Zhang, Hongzhi Cui, Guiqing Cheng, Jian Tian
    Chinese Chemical Letters. 2021, 32(11): 3501-3504.

    Recently, widespread attention has been devoted to the typical layered BiOCl or BiOBr because of the suitable nanostructure and band structure. However, owing to the fast carrier recombination, the photocatalytic performance of BiOX materials is not so satisfactory. Loading 1T phase WS2 nanosheets (NSs) onto Bi5O7Br NSs can improve the photocatalytic N2 fixation activity. Among these, the obtained 1T-WS2@Bi5O7Br composites with optimum 5% 1T-WS2 NSs display a significantly improved photocatalytic N2 fixation rate (8.43 mmol L-1h-1g-1), 2.51 times higher than pure Bi5O7Br (3.36 mmol L-1h-1g-1). And the outstanding stability of 1T-WS2@Bi5O7Br-5 composites is also achieved. Exactly, the photoexcited electrons from Bi5O7Br NSs are quickly transferred to conductive 1T phase WS2 as electron acceptors, which can promote the separation of carriers. In addition, 1T-WS2 NSs can provide abundant active sites on the basal and edge planes, which can promote the efficiency of photocatalytic N2 fixation. This work offers a novel solution to improve the photocatalytic performance of Bi5O7Br NSs.

  • Peng Jing, Boyuan Wu, Zongsu Han, Wei Shi, Peng Cheng
    Chinese Chemical Letters. 2021, 32(11): 3505-3508.

    The conversion of CO2 under mild condition is of great importance because these reactions involving CO2 can not only produce value-added chemicals from abundant and inexpensive CO2 feedstock but also close the carbon cycle. However, the chemical inertness of CO2 requires the development of high-performance catalysts. Herein, Ag nanoparticles/MIL-100(Fe) composites were synthesized by simple impregnation-reduction method and employed as catalysts for the photothermal carboxylation of terminal alkynes with CO2. MIL-100(Fe) could stabilize Ag nanoparticles and prevent them from aggregation during catalytic process. Taking the advantages of photothermal effects and catalytic activities of both Ag nanoparticles and MIL-100(Fe), various aromatic alkynes could be converted to corresponding carboxylic acid products (86%–92% yields) with 1 atm CO2 at room temperature under visible light irradiation when using Ag nanoparticles/MIL-100(Fe) as photothermal catalysts. The catalysts also showed good recyclability with almost no loss of catalytic activity for three consecutive runs. More importantly, the catalytic performance of Ag nanoparticles/MIL-100(Fe) under visible light irradiation at room temperature was comparable to that upon heating, showing that the light source could replace conventional heating method to drive the reaction. This work provided a promising strategy of utilizing solar energy for achieving efficient CO2 conversion to value-added chemicals under mild condition.

  • Danlin Bu, Yu Zhou, Chang Yang, Hengyu Feng, Chunxia Cheng, Mengjie Zhang, Zice Xu, Linghan Xiao, Yujing Liu, Zhenai Jin
    Chinese Chemical Letters. 2021, 32(11): 3509-3513.

    At present, frequent outbreaks of bacteria and viruses have seriously affected people's normal lives. Therefore, the study of broad-spectrum antibacterial nanocomposites is very promising. However, most antibacterial materials have some disadvantages, such as single bactericidal mechanisms and unrepeatable use. Based on the current situation, a kind of nanocomposite with three structures of graphene oxide (GO), quaternary ammonium salt (QAs) and N-halamine was prepared, which showed synergistic effect to improve antibacterial activity and combined with a variety of sterilization mechanisms. Meanwhile, GO can provide richer ways of sterilization and high specific surface area, which is conducive to the grafting of quaternarized N-halamine. The advantages of physical sterilization of GO, charge adsorption of QAs, reuse of N-halamine and efficient sterilization are fully utilized. The results showed that the quaternarized N-halamine-grafted GO was obtained successfully. GO grafted with quaternarized N-halamine polymer showed strong speedy bactericidal activity against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus) (99%). It had good storage and regeneration properties.

  • Qing Yu, Yunyun Liu, Jie-Ping Wan
    Chinese Chemical Letters. 2021, 32(11): 3514-3517.

    The perfluoroalkylsulfonylation (CF3SO2, C2F5SO2 and CHF2SO2) in the enaminone CH bonds has been developed simply via the promotion of molecular iodine by using stable and cheap sodium perfluoroalkyl sulfinates as coupling partners. The stereoselective synthesis of E-configurated α-perfluoroalkylsulfonyl enaminones has been realized via unprecedented CH bond elaboration and CC double bond configuration inversion by free radical process.

  • Xin Huang, Yingying Xu, Jianglian Li, Ruizhi Lai, Yi Luo, Qiantao Wang, Zhongzhen Yang, Yong Wu
    Chinese Chemical Letters. 2021, 32(11): 3518-3521.

    A new strategy is developed for the synthesis of 1-aminoisoquinoline derivatives. This Rh(Ⅲ)-catalyzed [4 + 2] annulation reaction employs benzamidines as efficient directing groups and the vinylene carbonate as an acetylene surrogate. Additionally, the reaction features broad substrate scopes and good yields, only producing carbonate anion as byproduct.

  • Ying Xiong, Chao Huang, Hongjuan Liu, Rui Yi, Bi-Xue Zhu, Xin-Long Ni
    Chinese Chemical Letters. 2021, 32(11): 3522-3525.

    The synthesis of cyclopolymers upon controlling the degree of macrocyclic polymerization, followed by the discovery of new properties has attracted increasing attention in supramolecular chemistry. Herein, a Schiff-base condensation method performed at room temperature was used to control the formation of [1 + 1] and [2 + 2] macrocycles. In pure MeOH, the isomer [1 + 1] macrocycles were synthesized and organic particles such as dendritic, rods, and solid microspheres were directly precipitated from the reaction solution. The [1 + 1] macrocycles can be efficiently converted into their corresponding [2 + 2] macrocycles accompanied by the tunable morphology of the organic particles when n-hexane was added to the MeOH solution. Further studies showed that these organic particles have potential application toward the selective removal of Cd2+ ions with different adsorption ability in MeOH solution.

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