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中国化学快报(英文版)
中国化学快报(英文版)

梁晓天

月刊

1001-8417

cclbj@imm.ac.cn

010-63165638

100050

北京市先农坛街1号

中国化学快报(英文版)/Journal Chinese Chemical LettersCSCDCSTPCD北大核心SCI
查看更多>>本刊是由中国科协主管、中国化学会主办、中国医学科学院药物所承办的学术期刊,是由著名化学家梁晓天院士主编。是中国化学界通向世界的窗口,内容覆盖化学全领域。本刊的办刊宗旨是“新、快、准”,我们将坚持这个宗旨,力求及时反映化学研究中各个相关领域内的最新进展及热点问题,主要读者群是科研人员、研究生、大学教师。现已被国内外多家数据库收录,如SCI Search、Chemical Abstract、Research Alert、Chemistry Citation Index、《日本科技文献速报》、万方数据数字化期刊群、中国学术期刊过刊全文数据库、中国学术期刊(光盘版)、中国学术期刊文摘、中文期刊全文数据库、俄罗斯Рж期刊源等。
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    Gelation mechanisms of gel polymer electrolytes for zinc-based batteries

    Mengjun SunZhi WangJvhui JiangXiaobing Wang...
    97-116页
    查看更多>>摘要:Zinc-based batteries(ZBs)have been deemed as a potential substitute for lithium-ion batteries due to its unique advantages of abundant resources,low cost and acceptable energy density.Despite great progress in designing electrode materials has been made,the development of high-performance ZBs still remain challenges,such as the dendrite growth of zinc anode,hydrogen evolution reaction,limited electrochem-ical stability window,water evaporation and liquid leakage.Gel polymer electrolytes(GPEs),including hydrous GPEs with low content of active water and anhydrous GPEs without the presence of water,are proposed to avoid these problems.Furthermore,employing GPEs is conductive to fabricate flexible de-vices owing to the good mechanical strength.To date,most of researches focus on discovering new GPEs and exploring its application on flexible or wearable devices.Recent reviews also have outlined the poly-mer matrixes and advances of GPEs in various battery systems.Given this,herein,we seek to summarize the gelation mechanisms of GPEs,involving physical gel of polymer,chemical crosslinking of polymer and chemical polymerization of monomers.Peculiarly,the preparation methods are also classified.In addition,not only the features and central conundrum of GPEs are analyzed but also the corresponding strategies are discussed,contributing to design GPEs with ideal properties for high-performance ZBs.

    Advanced development of grain boundaries in TMDs from fundamentals to hydrogen evolution application

    Ziyang YinLingbin XieWeinan YinTing Zhi...
    117-129页
    查看更多>>摘要:Grain boundary(GB),as a kind of lattice defect,widely exists in two-dimensional transition metal dichalcogenides(2D TMDs),which has complex and diverse influences on the physical/chemical prop-erties of 2D TMDs.GBs are universally considered to be a double-edged sword,although some electrical and mechanical properties of 2D TMDs would be adversely affected leading to the reduced overall qual-ity,certain structure-oriented applications could be realized based on its unique properties.In this review,we first detailed the atomic structure characteristics of GBs and the corresponding techniques,then we systematically summarized the methods of introducing GBs into 2D TMDs.Next,we expounded unique electrical,mechanical,and chemical properties of the GBs in 2D TMDs and clarified its internal relation-ship with the atomic structure.Moreover,the application of GB structure in hydrogen evolution reaction(HER)is also discussed.In the end,we make a conclusion and put forward outlooks,hoping to further promote the basic research of GB and boost the wide application of 2D TMDs.

    Elucidating ligand effects in rhodium(Ⅲ)-catalyzed arene-alkene coupling reactions

    Kongchuan WuDandan LuJianbin LinTing-Bin Wen...
    130-134页
    查看更多>>摘要:Rhodium(Ⅲ)-catalyzed C-H couplings of arenes with alkenes are among the most powerful methods for C-C bond formation.For these transformations,subtle manipulation of ancillary ligands can lead to dramatic changes in reactivity and selectivity.However,detailed mechanistic studies concerning the ligand effects are rare.In this study,we investigated the origin of ligand-controlled product-selectivity in rhodium(Ⅲ)-catalyzed C-H couplings of arenes with alkenes,using a series of well-defined[CpⅩRhⅢ]complexes that feature electronically or sterically distinct CpⅩ(Cp(η5-C5H5),CpCF3(η5-C5Me4CF3)and Cp*(η5-C5Me5))ligands.A combination of experimental and theoretical investigations showed that(ⅰ)rhodium hydride species containing the electron rich Cp*ligand can undergo reinsertion of the alkene,thereby allowing rhodium-walking,(ⅱ)rhodium hydride species involving the electron-deficient Cp or CpCF3 ligands prefer reductive elimination rather than alkene insertion.These findings offer valuable in-sights on future rational catalyst design for selective arene-alkene cross coupling reactions.

    Asymmetric alkenylation reaction of benzoxazinones with diarylethylenes catalyzed by B(C6F5)3/chiral phosphoric acid

    Zhen LiuZhi-Yuan RenChen YangXiangyi Shao...
    135-140页
    查看更多>>摘要:Catalytic enantioselective alkenylation is an efficient method to construct chiral alkene molecules,but the asymmetric alkenylation of simple alkenes catalyzed by metal-free catalysts remains an elusive chal-lenge.Herein,we reported an asymmetric alkenylation of benzoxazinones with diarylethylenes by uti-lizing a B(C6F5)3/chiral phosphoric acid catalyst.A broad of benzoxazinones and diarylethylenes with electron-withdrawing and electron-donating groups were tolerated(up to 95%yield and 97.5∶2.5 e.r.)in the methodology under mild reaction conditions.Moreover,the synthetic utility was confirmed by the scaled-up reaction and transformations of the products.The mechanism was preliminarily explored by control reactions,nonlinear effect experiment and DFT calculations.

    Cu-catalyzed regioselective diborylation of 1,3-enynes for the efficient synthesis of 1,4-diborylated allenes

    Wujun JianMong-Feng ChiouYajun LiHongli Bao...
    141-144页
    查看更多>>摘要:Borylation of 1,3-enynes with bis(boronate)compounds often ends up with the formation of hydrobo-rylated products,leaving the diborylation of 1,3-enynes for the formation of 1,4-diborylated allenes to be challenging.Herein,a copper-catalyzed chemo-,regio-,and stereo-selective diborylation of 1,3-enynes for the efficient construction of 1,4-diborylated allenes under base-free conditions was reported.A wide range of 1,3-enynes bearing various functional groups can participant in the reaction and afforded the corresponding 1,4-diborylated allenes in good to excellent yields,which was enabled by the protocol of Bpin to BF3K conversion.the borylcopper species was supposed to selectively attack the C-C triple bond of the 1,3-enynes.

    An improved installation of 2-hydroxy-4-methoxybenzyl(iHmb)method for chemical protein synthesis

    Ying LiLong-Jie WangYong-Kang ZhouJun Liang...
    145-150页
    查看更多>>摘要:The 2-hydroxy-4-methoxybenzyl(Hmb)backbone modification can prevent amide bond-mediated side-reactions(e.g.,aspartimide formation,peptide aggregation)by installing the removable Hmb group into a peptide bond,thus improving the synthesis of long and challenging peptides and proteins.However,its use is largely precluded by the limited Hmb's installation sites.In this report,an improved installa-tion of Hmb(iHmb)method was developed to achieve the flexible installation and the convenient re-moval of Hmb.The iHmb method involves two critical steps:(1)oxidative diazotization of the readily in-stalled 2-hydroxy-4-methoxy-5-amino-benzyl(Hmab)to give 2-hydroxy-4-methoxy-5-diazonium-benzyl(Hmdab)by combining soamyl nitrite(1AN)/HBF4,and(2)reductive elimination of Hmdab to give the de-sired Hmb by 1,2-ethanedithiol(EDT).The iHmb method enables the installation of Hmb at any primary amino acid including the highly sterically hindered amino acids(e.g.,valine and isoleucine).The practical-ity and utility of the iHmb method was demonstrated by one-shot solid-phase synthesis of a challenging aspartimide-prone peptide,the mirror-image version of a hydrophobic peptide and a long-chain peptide up to 76-residue.Furthermore,the iHmb method can be utilized to facilitate chemical protein ligation,as exemplified by the synthesis of the single-spanning membrane protein sarcolipin.The iHmb method expands the toolkit for peptide synthesis and ligation and facilitates the preparation of peptides/proteins.

    S-(1,3-Dioxoisoindolin-2-yl)O,O-diethyl phosphorothioate(SDDP):A practical electrophilic reagent for the phosphorothiolation of electron-rich compounds

    Ze-Yuan MaMei XiaoCheng-Kun LiAdedamola Shoberu...
    151-154页
    查看更多>>摘要:An efficient synthesis of the electrophilic reagent,S-(1,3-dioxoisoindolin-2-yl)O,O-diethyl phosphoroth-ioate(SDDP)is described.Moreover,the synthetic applications of SDDP wherein the transfer of the SP(O)(OEt)2 moiety occurs were investigated.In this manner,SDDP underwent facile SP(O)(OEt)2 transfer with electron-rich substrates such as ketones,indoles,and thiols to form α-phosphorothiolated ketones,3-phosphorothiolated indoles and S-phosphorothiolated thioethers,respectively.

    Convergent synthesis and immunological study of oligosaccharide derivatives related to galactomannan from Antrodia cinnamomea

    Shuying LiWeiwei ZhuGeXuan SunChongzhen Sun...
    155-160页
    查看更多>>摘要:The galactomannan from Antrodia cinnamomea(AC)is characterized as one of the important bioactive components that exhibits potential immunostimulatory propriety.The biological function of its corre-sponding oligosaccharide fragments has not been revealed yet.In this study,we reported the first chem-ical synthesis of the series of oligosaccharide fragments related to AC galactomannan via the convergent glycosylation strategy.The preliminary immunological evaluation of these synthesized AC oligosaccha-rides disclosed that the backbone tetrasaccharide 1d showed the best immunomodulatory ability on en-hancing proliferation,phagocytosis and cytokines secretion of Raw264.7 macrophages in vitro,indicating its immense potential as an immunostimulant candidate.

    Enhancing hydrolytic stability of dynamic imine bonds and polymers in acidic media with internal protecting groups

    Hang ChenChengzhi CuiHebo YeHanxun Zou...
    161-165页
    查看更多>>摘要:Imine bonds are among the most explored building motifs in dynamic chemistry,polymers,and materials,and yet,their acid-resistance remains a longstanding issue.Herein we demonstrate a concept of internal protecting groups for improving the kinetic stability of dynamic imine bonds and polymers.Systematic examination of structure-reactivity relationship of a series of aldehydes/imines bearing a neighboring car-boxyl allowed uncovering of required structural features for dynamically masking imine bonds with cyclic structures.Mechanistic studies indicated that noncovalent interactions along with sterics control the ring-chain equilibrium and the stability of imine bonds.The incorporation of internal protecting groups into imine polymers further enabled their controlled stability in acidic media.Moreover,a combination of dy-namic covalent network and coordination supramolecular network provided a facile means for the mod-ulation of luminescent and mechanical properties of polymers.The strategies and results reported should be beneficial to molecular assemblies,dynamic polymers,biological delivery,and intelligent materials.

    Dihydroanthracene bridged bis-naphthopyrans:A multimodal chromophore with mechano-and photo-chromic properties

    Yanbing ShenYuan YuanYaxin WangXiaonan Ma...
    166-170页
    查看更多>>摘要:Mechanochromophores based on bichromic molecular switches,such as bis-naphthopyanes,allow multi-modal mechanochromic behavior beyond the typical binary response from single chromophores,which is important for distinguishing between multiple stress states through discrete changes in color.Sponta-neously generated persistent and distinguishable multi-colors from activated bis-naphthopyanes remain challenging.And the versatility of bis-mechanophore design for advanced optical molecular systems and the fundamental insights into the corresponding mechano-reactivity are not enough.Here,we identify a dihydroanthracene bridged bis-naphthopyrans as a multimodal mechanochromophore in polymers.Bridg-ing two pyrans with the sterically constrained dihydroanthracene is helpful to control the steric effect for the favorable formation of a distinctly appreciable bis-merocyanine(bis-MC)product.By varying the length of the polymer chains,the force delivered to the mechanophore is modulated,resulting in a gradient change in the relative distribution of two distinctly colored MC products and a multicolor mechanochromism.Mechanical activation of this bis-naphthopyanes proceeds via a mechanistically dis-tinct pathway compared to the photochemical process.In addition,the bulk films can also achieve pro-nounced color changes when subjected to mechanical force.This study thus further expands the molecu-lar diversity of mechanochromophores and tune the multimodal switch properties of bis-naphthopyrans based polymers.