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  • Xueting Zhao, Yuanyuan Jiang, Lijuan Cheng, Youyou Lan, Tingyuan Wang, Jiefeng Pan, Lifen Liu
    Chinese Chemical Letters. 2022, 33(8): 3859-3864.

    Superwetting membranes have emerged as promising materials for the efficient treatment of oily wastewater. Typically, superwetting membranes can be developed by ingeniously chemical modification and topographical structuration of microporous membranes. Herein, we report the hierarchical assembly of metal-phenolic-polyplex coating to manipulate membrane surface superwettability by integrating metal-phenolic (FeⅢ-tannic acid (TA)) assembly with polyplex (tannic acid-polyethylenimine (PEI)) assembly. The proposed Fe-TA-PEI coating can be deposited on microporous membrane via simply dipping into FeⅢ-TA-PEI co-assembly solution. Based on the catechol chemistry, the coordination complexation of FeⅢ and TA develops metal-phenolic networks to provide hydrophilic chemistries, and the electrostatic complexation of TA and PEI generates nanoconjugates to impart hierarchical architectures. Benefiting from the synergy of hydrophilic chemistries and hierarchical architectures, the resulting PVDF/Fe-TA-PEI membrane exhibits excellent superhydrophilicity (~0°), underwater superoleophobicity (~150°) and superior anti-oil-adhesion capability. The superhydrophilicity of PVDF/Fe-TA-PEI membrane greatly promotes membrane permeability, featuring water fluxes up to 5860 L m−2 h−1. The underwater superoleophobicity of PVDF/Fe-TA-PEI membrane promises potential flux (3393 L m−2 h−1), high separation efficiency (99.3%) and desirable antifouling capability for oil-in-water emulsion separation. Thus, we highlight the reported hierarchical metal-phenolic-polyplex assembly as a straightforward and effective strategy that enables the synchronous modulation of surface chemistry and topography toward superwetting membranes for promising high-flux and antifouling oil-water separation.

  • Jie Shen, Juan Chen, Dong Wang, Zhengjie Liu, Guangmei Han, Bianhua Liu, Mingyong Han, Ruilong Zhang, Guodong Liu, Zhongping Zhang
    Chinese Chemical Letters. 2022, 33(8): 3865-3868.

    Nuclear RNA export into the cytoplasm is one of the key steps in protein expression to realize biological functions. Despite the broad availability of nucleic acid dyes, tracking and quantifying the highly dynamic process of RNA export in live cells is challenging. When dye-labeled RNA enters the cytoplasm, the dye molecules are released upon degradation of the RNA, allowing them to re-enter the cell nucleus. As a result, the ratio between the dye exported with RNA into the cytoplasm and the portion staying inside the nucleus cannot be determined. To address this common limitation, we report the design of a smart probe that can only check into the nucleus once. When adding to cells, this probe rapidly binds with nuclear RNAs in live cells and reacts with intrinsic H2S. This reaction not only activates the fluorescence for RNA tracking but also changes the structure of probe and consequently its intracellular localization. After disassociating from exported RNAs in cytoplasm, the probe preferentially enters lysosomes rather than cell nucleus, enabling real-time quantitative measurement of nuclear RNA exports. Using this probe, we successfully evaluated the effects of hormones and cancer drugs on nuclear RNA export in live cells. Interestingly, we found that hormones inhibiting RNA exports can partially offset the effect of chemotherapy.

  • Tiantian Si, Xiaofeng Lu, Haixia Zhang, Shuai Wang, Xiaojing Liang, Yong Guo
    Chinese Chemical Letters. 2022, 33(8): 3869-3872.

    Here, silica microspheres were decorated with two-dimensional metal–organic frameworks (2D MOFs) nanosheets and ionic liquids, and evaluated as the mixed-mode stationary phase for chromatographic separation. The ionic liquids were used to assist the synthesis of 2D MOFs nanosheets, and also acted as adhesives among the nanosheets and silica. In contrast with the 2D MOFs-based column without ionic liquids and commercial columns, the prepared column exhibited enhanced chromatographic separation performance for partially hydrophilic compounds such as alkaloids, sulfonamides and antibiotics, etc. In addition to excellent chromatographic repeatability and stability, it has also been verified that the composites could be easily and repeatedly prepared. The relative standard deviation of the retention time of the same type of analyte between the three batches of materials was ranging from 0.21% to 1.7%. In short, these results indicated that the synthesized composites were promising separation material for liquid chromatography, which made it possible to broaden the application of 2D MOFs in the field of chromatography.

  • Jing-Jing Zhang, Si-Ying Wang, Pan Zhang, Shu-Chen Fan, Hai-Tao Dai, Yin Xiao, Yong Wang
    Chinese Chemical Letters. 2022, 33(8): 3873-3878.

    Chiral recognition of essential amino acids (EAAs) is a huge challenge that keeps plaguing analytical scientists due to their cryptochirality and limited steric interaction sites. Inspired by the superior enantioselectivity of functional supramolecular cyclodextrins (CDs) and strong signal amplification ability of field effect transistors (FETs), this work firstly reports a cationic supramolecular charge switch for facile enantiodiscrimination of EAAs based on extended-gate organic FET (EG-OFET). The cationic phenylcarbamoylated-CD single isomer acts as a charge switch via interacting with different enantiomers and the weak stereo-differentiation intermolecular interaction signals between the cationic perphenylcarbamoylated CDs and EAAs on the EG can be strongly and rapidly amplified through an OFET. Efficient chiral differentiation of six EAAs, including phenylalanine, tryptophan, leucine, isoleucine, lysine and valine, are successfully achieved without any derivation process and the detection limit for D-phenylalanine is down to 10−13 mol/L. We believe that this study provides a new and facile sensing perspective for natural amino acids and may afford deeper understanding of molecular chirality.

  • Yongchao Song, Dongdong Wang, Zehua Li, Lirong Wang, Chuan Fan, Xuecheng He, Tailin Xu, Xueji Zhang
    Chinese Chemical Letters. 2022, 33(8): 3879-3882.

    The multiple sensing provides booming options to eliminate interference and ensure the accuracy of detection by mutually coupling and validating multiple data sets. Here, we integrate the jigsaw-like multifunctional mini-pillar platform to perform multi-mode (electrochemical, fluorescence, surface-enhanced Raman scattering (SERS) and colorimetric) sensing in individual microdroplets. Each mini-pillar connector can parallelize together by specific concave-convex interface to form integrated jigsaw-like platform for multi-mode sensing, and each specific mini-pillar can be modified into the individual sensing unit to read the prescribed signals. We successfully implemented electrochemical, fluorescence, SERS and colorimetric detection by multiple signals coupling to reduce the false positive analysis. Such platform brings a promising clue of in-situ analysis and point-of-care testing for disease diagnosis and health monitoring.

  • Xiao Wang, Kaixiang Zou, Weijing Wu, Yuanfu Deng, Guohua Chen
    Chinese Chemical Letters. 2022, 33(8): 3883-3888.

    Designing a carbon material with a unique composition and surface functional groups for offering high specific capacity in a wide voltage window is of great significance to improve the energy density for the supercapacitor in a cheap and eco-friendly aqueous electrolyte. Herein, we develop an efficient strategy to synthesize a N, O co-doped hierarchically porous carbon (NODPC-1.0) with moderate specific surface area and pore volume as well as rich heteroatoms using a deep eutectic solvent (DES) as an activator. It is found that NODPC-1.0 with a large proportion of pseudocapacitive functional groups (pyrrole-N, pyridine-N and carbonyl-quinone) can work stable in an acidic 2 mol/L Li2SO4 (pH 2.5) electrolyte, exhibiting specific capacities of 375 and 186 F/g at the current densities of 1.0 and 100 A/g, respectively. Also, the assembled symmetric capacitor using the NODPC-1.0 as the active material and 2 mol/L acidic Li2SO4 (pH 2.5) as the electrolyte shows an outstanding energy density of 74.4 Wh/kg at a high power density of 1.44 kW/kg under a broad voltage window (2.4 V). Relevant comparative experiments indicate that H+ of the acidic aqueous electrolyte plays a crucial part in enhancement the specific capacity, and the abundant pseudocapacitive functional groups on the surface of the NODPC-1.0 sample play the key role in the improvement of electrochemical cycle stability under a broad voltage window.

  • Jianmin Yuan, Nan Qin, Yanyan Lu, Liming Jin, Junsheng Zheng, Jim P. Zheng
    Chinese Chemical Letters. 2022, 33(8): 3889-3893.

    Lithium-ion capacitor (LIC), which combines the advantages of lithium-ion battery (LIB) and electrical double layer capacitor (EDLC), has a rapid development during last decade, however, the poor low temperature performance still limits its application. In this paper, three electrolyte additives including vinylene carbonate (VC), fluoroethylene carbonate (FEC) and 1,3,2-dioxathiolane 2,2-dioxide (DTD) have been utilized and their effects on the rate performance of hard carbon (HC) anode of LIC at various temperatures ranging from 25 ℃ to −40 ℃ have been well evaluated. The cell containing FEC shows the best rate performance at various temperatures and has the charge and discharge capability even at −40 ℃. For HC anode, the charge transfer impedance (RCT) increases exponentially at low temperature, while the equivalent series resistance (Rs) and the impedance of solid electrolyte interface (SEI) increase relatively few. At low temperatures, the effect of FEC may be mainly reflected in its effect on the charge transfer process.

  • Menghan Ge, Xiaoyu Zhou, Yinping Qin, Yang Liu, Jingjing Zhou, Xiaolei Wang, Bingkun Guo
    Chinese Chemical Letters. 2022, 33(8): 3894-3898.

    The lithium dendrite growth is still a serious challenge and impeding the realistic applications of all-solid-state lithium batteries. In view of the amide containing sediment layer can be stable on lithium/cathodes, a composite polymer electrolyte with amide-based matrix is in-situ built on porous electrodes. With the introduction of amide, the polymer electrolyte presents excellent ability to inhibit lithium dendrite growth and makes the Li/Li symmetric battery stably work for 500 h with a good ionic conductivity of 4.25 × 10−5 S/cm at 40 ℃. The solid electrolyte also shows a wide electrochemical stable window and good interface contact with the porous cathode. Utilizing this composite polymer electrolyte, the all-solid-state Li/LiFePO4 battery shows an initial discharge capacity of 146.5 mAh/g at 0.1 C under 40 ℃ and remains 81.4% in 100 cycles. The polymer electrolyte also can present better properties after modification. These results demonstrate that the presented PA-based composite polymer electrolyte could be served as a good electrolyte candidate for all-solid-state lithium-ion batteries.

  • Mengyuan Cheng, Yufeng Liu, Weixin Du, Jingwen Shi, Junhua Li, Haiying Wang, Ke Li, Guoping Yang, Dongdi Zhang
    Chinese Chemical Letters. 2022, 33(8): 3899-3902.

    Two novel uranium-containing selenotungstates Na3[H19(UO2)2(μ2-O)(Se2W14O52)2]·41H2O (U2) and (NH4)10[H4(SeO)2(UO2)2(H2O)2(H2Se2W14O52)(Se2W14O52)]·66H2O (Se2U2) based on the {Se2W14O52} unit were successfully prepared and fully characterized. To our knowledge, the uranium is firstly introduced into the selenotungstates. Moreover, it is notable that U2 exhibits excellent Lewis acid-base catalytic activities in the condensation cyclization of sulfonyl hydrazides with diketones to synthesize polysubstituted pyrazoles. All the desired products were obtained in moderate to good yields (up to 99%).

  • Guangying Zhang, Xu Liu, Peng Yu, Di Shen, Bowen Liu, Qiwen Pan, Lei Wang, Honggang Fu
    Chinese Chemical Letters. 2022, 33(8): 3903-3908.

    Fe-N-C structures have been considered as a candidate to replace noble metal catalysts towards oxygen reduction reaction (ORR) due to their excellent electrocatalytic activity and durability. Herein, a zinc-mediated synthesis strategy is proposed for N-doped graphitic porous carbon encapsulated uniform dispersed Fe3C nanoparticles coupled with atomically dispersed Fe-Nx moieties (NPC/Fe-N-C) derived from biomass coconut shell. The introduction of zinc species could be conductive to the dispersion of iron species and formation of porous structures. Density functional theory calculations demonstrate that the N-doped carbon coating structures can weaken the oxygen intermediates adsorption energy barrier of Fe3C. Beside, the graphitic carbon could promote the electron transfer during the electrochemical reaction. These special structures enable NPC/Fe-N-C to have excellent ORR activity with an Eonset of 1.0 V, which is much better than Pt/C. Furthermore, the zinc-air battery assembled by pairing NPC/Fe-N-C with a high-efficiency oxygen evolution reaction (OER) catalyst can continuously and stably operate a charge-discharge potential gap of 0.8 V at 10 mA/cm2 for more than 600 h. More importantly, the assembled batteries could drive overall water splitting device, realizing the effective energy conversion.

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