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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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    Evaluating the tumor stratification with a lysosomal pH sensitive-probe by fluorescence lifetime imaging

    Jun YanXing LiangQian ZhangLuolin Wang...
    262-267页
    查看更多>>摘要：Owing to the anaerobic metabolism in the tumor,abundant acidic metabolites are produced and accu-mulated in the cells.Therefore,the cells in different tumor layers are directly linked to the pH micro-environment.Nevertheless,due to the lack of robust tools,the high-efficient evaluation of the acidic micro-environment of tumor stratification faces the challenge of accurate diagnosis.We designed a new pH sensitive fluorescent lifetime probe target to lysosomes.As we expected,the fluorescence lifetime of PLN possesses a good linear fit to the pH value,which could detect the pH change at a single lysosome level in real time,and then evaluate the different acidity of tumor stratification.The probe PLN is suc-cessfully used to evaluate the tumor stratification by fluorescence lifetime imaging microscopy(FLIM)for the first time,which is of great significance in the preoperative diagnosis of clinical tumor treatment or evaluation of drug delivery effect.
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    Anion-induced differential assembly and structural transformation of supramolecular coordination cages

    Shao-Ping ZhengYao-Wei XuPei-Yang SuChen-Hui Liu...
    268-272页
    查看更多>>摘要：The intimate host-anion interactions will regulate thermodynamics and kinetics in the self-assembly of cationic cages mimicking biological counterparts.Herein,we report construction and transformation of three Pd(Ⅱ)-based metal-organic cages(MOCs)depending on different anions.Stoichiometric conversions of the lantern-shaped MOC-34 into either octahedral MOC-35 or tricapped trigonal prism MOC-36 are induced by BF4-or NO3-,respectively.MOC-36 is kinetically favored and can undergo quantitative con-version to the thermodynamically preferred MOC-35 upon heating,accelerated by excess BF4-to motivate dissociative dynamics of Pd-vertices and lower activation barrier of cage transformation.The guest encap-sulation behaviors of MOC-35 and MOC-36 have also been tested.These results manifest a significance of host-anion dynamics beyond complementary anion template,shedding light on the understanding of intricate anion recognition in nature.
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    Selective synthesis and physical properties of a bismacrocycle:Cycloparaphenylene-pillar[5]arene

    Yu ZhouGuilin ZhuangPingwu Du
    273-276页
    查看更多>>摘要：Macrocyclic materials have attracted much attention due to their particular chemical and physical proper-ties.Herein we report the precise synthesis and characterization of a new bismacrocycle structure base on cycloparaphenylene(CPP)and pillar[5]arene,named cycloparaphenylene-pillar[5]arenes(CPPn[5]).The bismacrocycle was fully characterized by NMR and HR-MS.The photophysical properties of CPPn[5]were investigated by UV-vis,and the maximum absorption peak was located at 331 nm,which was consis-tent with density functional theory(DFT)calculations.The fluorescence spectrum was further studied and the emission peak was maximized at 458 nm.The computational results indicate the strain energy of CPPn[5]is 27.80 kcal/mol and the HOMO-LUMO gap is 3.39 eV Notably,CPPn[5]showed interesting supramolecular properties.
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    Cobalt-catalyzed deoxygenative borylation of diaryl ketones

    Longqing LiuBing ZhangYu LiuJinbo Zhao...
    277-281页
    查看更多>>摘要：Geminal diboronates and diarylmethyl boronates are versatile building blocks in synthetic chemistry.We here reported a highly efficient approach for the synthesis of gem-bisborylalkanes and diarylmethyl boronates via cobalt-catalyzed deoxygenative borylation of diaryl ketones.This borylation protocol is compatible with a broad range of functionalized aryl groups,providing access to a wide array of boronic esters.The resulting boronic esters can be further transformed to various cross-coupling products and TPEs that represent important structural motifs in organic chemistry and materials science.
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    Zwitterionic ring-opening polymerization of macrocyclic ethyleneoxy-substituted carbonate:Access to cyclic PEG-like polycarbonate

    Jin HuangJinwen LiRui YanYuanyuan Qu...
    282-286页
    查看更多>>摘要：The innovation in polymer design to rival conventional polyethylene glycol(PEG)is an important ap-proach to achieving a more sustainable society.Here,cyclic PEG-like polycarbonates having high molec-ular weight(4.4-49.5 kg/mol)were enabled through zwitterionic ring-opening polymerization(ZROP)of macrocyclic carbonates(MCs)mediated by N-heterocyclic carbene(NHC).The thermodynamic behavior of polymerization depends on the ring size of monomers.During this process,the ZROP of 11-membered MC was driven by the change of enthalpy(ΔHp)which differed from the ZROP of 14-membered MC driven by the entropic change(ΔSp).Cyclic polycarbonates depicted improved thermostability(Td5％≥ 204 ℃)and higher glass transition temperatures(Tg＞-40 ℃)in comparison to their linear analogues(Td5％≤ 185 ℃,Tg～-50 ℃).In addition,the mechanism of ZROP of MC was addressed through computational study.A distinct mechanism of polymerization distinguishable from the well-known NHC-mediated ZROP of cyclic esters was revealed,where the zwitterion from nucleophilic addition to MC,i.e.tetrahedral intermediate,cannot be ring-opened probably due to the delocalization of negative charge on the carbonate group,but serves as an active center for the polymerization.In comparison to PEG,the attained polymer demon-strated comparable hydrophilic and biocompatible properties,as revealed by the results of contact angle and in vitro cytotoxicity studies,suggesting that cyclic polycarbonate hold the promise as the alternative of PEG.
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    Rhodium-catalyzed addition reactions of benzylic C-H bonds to cyclic N-sulfonyl ketimines via π-coordination

    Yuntong LiHang Shi
    287-291页
    查看更多>>摘要：Mannich-type reactions are a widely used method for the synthesis of amines due to the readily avail-ability of nucleophiles and electrophiles.However,the inclusion of alkylarenes instead of active carbon pronucleophiles such as aldehydes and ketones in these addition reactions has been a challenge due to the inherent difficulty of benzylic deprotonation.In this study,we present a novel approach for the con-struction of N-sulfonyl amines via rhodium-catalyzed addition of unbiased benzylic C-H bonds to cyclic N-sulfonyl ketamines through π-coordination.This strategy enables the synthesis of a diverse range of N-sulfonyl amines,and subsequent diversification of the addition products showcases the synthetic po-tential of this protocol.
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    Four-coordinate disilyl cobalt(Ⅱ)complexes with NHC ligation:Synthesis,characterization,and reactivity

    Lan ZhouDongyang WangChengbo YangLiang Deng...
    292-298页
    查看更多>>摘要：Silyl cobalt species are putative intermediates in cobalt-catalyzed transformations of hydrosilanes.However,their reactivity has remained poorly understood.Reported here is the investigation on four-coordinate disilyl Co(Ⅱ)complexes with N-hetereocyclic carbene ligation.The reactions of[(ICy)2Co(vtms)](ICy=1,3-dicyclohexylimidazol-2-ylidene,vtms=vinyltrimethylsilane)with pri-mary and secondary hydrosilanes(3 equiv.)furnish the four-coordinate disilyl complexes[trans-(ICy)2Co(SiHRR')2](SiHRR'=SiH2Mes,1;SiH2Ph,2;SiH2Cy,3;SiHPh2,4;SiHEt2,5)in moderate to good yields.The structures of 1,2 and 4 were established by single-crystal X-ray diffraction.Solution mag-netic susceptibility measurement and EPR spectroscopy indicate their low-spin nature(S=1/2).Reactiv-ity studies on 4 led to the establishment of the conversions of 4 to the disilyl dihydride Co(Ⅲ)complex[K(THF)][(ICy)2Co(H)2(SiHPh2)2]n(6)and the fluorosilyl Co(Ⅱ)complex[(ICy)2Co(THF)(SiFPh2)][BF4](7)when 4 was treated with excess amount of K and AgBF4,respectively,in THF.These conversions hint at the high activity of low-valent and high-valent disilyl cobalt species[trans-(ICy)2Co(SiHPh2)2]1-and[trans-(ICy)2Co(SiHPh2)2]2+.Complex 4 is reactive toward terminal alkynes,but inert toward alkenes and internal alkynes.The reactions of 4 with terminal alkynes CyC=CH and Me3SiC=CH(3 equiv.)yield the Co(Ⅱ)complexes[(ICy)2Co(C≡CCy)2](8)and[(ICy)2Co(C=CSiMe3)((SiMe3)C=CH2)](9),respectively,along with H2SiPh2 and alkynylsilanes RC=CSiHPh2(R=Cy,SiMe3),whereas the reaction with 4-CF3C6H4C≡CH(3 equiv.)produce[(ICy)2Co(C=CAr)((Ar)C=CH(SiHPh2)C=CHAr)](Ar=4-CF3C6H4)(10)and H2SiPh2.These reactions are proposed to involve σ-bond metathesis reactions between alkyne C(sp)-H bonds and Co-Si bonds in 4.Complexes 6-10 have been characterized by NMR spectroscopy,X-ray diffraction study,and elemental analysis.
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    Continuous-flow enzymatic synthesis of chiral lactones in a three-dimensional microfluidic reactor

    Xuelei DengMeng FanMiao WuXiaoyan Zhang...
    299-303页
    查看更多>>摘要：A new continuous-flow process for the enzymatic synthesis of optically pure γ-lactones,which are used as flavors and fragrances in the food and cosmetic industries,was developed in a three-dimensional microfluidic reactor.The microchannels(175 mm in length,0.9 mm in depth,and 1.72 mL in volume)were carved precisely inside a single borosilicate glass(90 mm × 75 mm × 12 mm)with ultrafast fem-tosecond laser micromachining.The flow field analysis and reaction simulation showed that the mix-ing of substrates and enzymes was enhanced,allowing the adjustment of residence time in a wide win-dow.SmCRV4,a carbonyl reductase with excellent catalytic activity and enantioselectivity toward γ/δ-keto acids,was employed for the asymmetric synthesis of various chiral lactones.30mmol/L(R)-y-decalactone(3g)can be obtained in 26 s with a space-time yield(STY)up to 16,877 g L-1 d-1,which is 14.4 times higher than the highest STY of batch reaction reported previously.This continuous-flow process was ap-plied to the synthesis of 6 chiral lactones.In addition,the scaled-up synthesis of 3g was carried out in 6 cascade microreactors continuously for 6h,demonstrating the feasibility and stability of the 3D continuous-flow process in enzymatic synthesis of optically pure compounds.
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    Germylene-Fe complexes caused by heterometallic coupling and investigation into the 3d-4p bonding

    Yingying QinYongmei KangLei ZhangJianping Sun...
    304-307页
    查看更多>>摘要：The interpretation of heterometallic bonding nature is a basic work of inorganic chemistry.By means of intermetallic substitution of germylene anions with iron halide complexes CpFe(CO)2I and β-diketiminato FeⅡ chloride,the ferrogermylene complexes 3a,3b and 4a were synthesized and structurally charac-terized.The structural and IR characterizations show the presence of the Ge←Fe π backbonding in molecules 3a,3b and 4a.The computational works on frontier molecular orbitals and their compari-son of energy states confirmed that σ donation and π backbonding are both weak in these molecules,despite three complexes have longer Ge-Fe bonds,whose strength decreases slightly with the degressive electron density around Fe environment in a sequence from 3a,3b to 4a.
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    A meso-molecular muscle based on copillar[5]arenes

    Yu YaoPeiling ZhangDan ZhouZhinan Lai...
    308-311页
    查看更多>>摘要：A meso-molecular muscle was prepared by capping the[c2]daisy chain based on a mono-functionalized copillar[5]arene with an imidazolium group in its axle.From its crystal structure,we observed that it was a cyclic dimer composed of two mirror image subcomponents,a pR-and a pS-copillar[5]arene.Their conformations were fixed by the doubly interlocked mechanical bond.By comparison of the 1H NMR and COSY spectra,we found that the length of this meso-molecular muscle could be controlled not only by the solvents,but also by the counter anions.
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