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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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    Construction of metallo-complexes with 2,2′:6′,2″-terpyridine substituted triphenylamine in different modified positions and their photophysical properties

    Shengwen GuanZhaotong WeiNingxu HanYude Wei...
    301-305页
    查看更多>>摘要：The stable coordinated metallo-complexes based on 2,2′:6′,2″-terpyridine(tpy)and its derivatives have been widely researched for various wide-ranging applications in photoelectronics,catalysis,sensor,pho-toluminescence,and so on.However,the most reported studies ignored the comprehensive comparison between structures modified by different positions and photoluminescence.Herein,we design a series of metallo-complexes which were assembled with tpy substituted triphenylamine(TPA)at different po-sitions and metal ions and explored their photophysical properties.In the solution state,MLE2 based on the 5,5″-positions modification showed the highest PLQYs and PL intensity.With the increase of solvent polarity,MLB2 exhibit the largest redshift.In the solid state,from MLA2 to MLE2,the emission colours are gradually red-shifted from yellow to red.The findings in this work may pave a new way to design functional metallo-complexes,not just for PL properties.
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    Theoretical perspectives on the reduction of Pu(Ⅳ)and Np(Ⅵ)by methylhydrazine in HNO3 solution:Implications for Np/Pu separation

    Xiaobo LiQunyan WuCongzhi WangJianhui Lan...
    306-312页
    查看更多>>摘要：Effective adjustment and control of the oxidation state of plutonium(Pu)and neptunium(Np)is an in-dispensable component of Np/Pu separation in spent nuclear fuel reprocessing.Some hydrazine deriva-tives including methylhydrazine(CH3N2H3)effectively achieves the reduction of Np(Ⅵ)to Np(Ⅴ)without reducing Pu(Ⅳ).Herein,we explored the reduction mechanisms of Pu(Ⅳ)and Np(Ⅵ)by CH3N2H3 in HNO3 solution using scalar-relativistic density functional theory.We elucidated the difference in the re-duction mechanism between Np(Ⅵ)and Pu(Ⅳ)ions by CH3N2H3.The energy barrier for the reduction of[NpⅥO2(H2O)5]2+ and[NpⅥO2(NO3)(H2O)3]+by CH3N2H3 is largely different due to the coordination of nitrate ion.Moreover,the energy barrier of the reduction of[NpⅥO2(H2O)5]2+ is apparently lower than that of[PuⅣ(NO3)2(H2O)7]2+,which is in line with the experimental observations.The results of Mayer bond order and localized molecular orbitals clarify the structural evolution of the reaction path-ways.Analysis of the spin density demonstrates that the first Np(Ⅵ)and Pu(Ⅳ)reduction belongs to the outer-sphere electron transfer and the second Np(Ⅵ)and Pu(Ⅳ)reduction is the hydrogen transfer.This study explains theoretically why CH3N2H3 reduces Np(Ⅵ)but not Pu(Ⅳ),and helps to design promising reductants for the Np/Pu separation in spent nuclear fuel reprocessing.
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    A nitroreductase-responsive nanoprobe with homogeneous composition and high loading for preoperative non-invasive tumor imaging and intraoperative guidance

    Jingqi XinShupeng HanMeichen ZhengChenfeng Xu...
    313-318页
    查看更多>>摘要：Tumor microenvironment(TME)-activatable probes have been proven to effectively increase signal-to-background ratios(SBRs)and improve the success rate of complete tumor resection.However,many fluo-rescence probes have to be loaded into a nanocarrier for tumor targeted delivery,which consequently en-counters poor drug loading,heterogeneous composition and non-encapsulated drug aggregates occurred during nanoformulation fabrications.Herein,a nitroreductase(NTR)-activated"OFF-ON"near-infrared flu-orescence nanoprobe,named NanoBodipy,was synthesized by the spontaneous self-assembling of NTR-responsive dye-polyethylene glycol(PEG)amphiphilic polymer in water.The NTR-responsive dye acted as the hydrophobic segment in the amphiphilic polymer,yielding a homogeneous composition and a high loading of 12.2 wt% (according to calculation)in the synthesized NanoBodipy.The synthesized NanoBod-ipy can efficiently accumulate in tumors via the enhanced permeability and retention(EPR)effect,en-abling non-invasive tumor-targeted fluorescence imaging and guiding complete tumor resection.Once the synthesized NanoBodipy entered the tumor cells,they dissociated and were activated by overexpressed NTR.With the real-time fluorescence guide of NanoBodipy,complete tumor resection surgery was per-formed successfully.
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    Engineered exosome hybrid copper nanoscale antibiotics facilitate simultaneous self-assembly imaging and elimination of intracellular multidrug-resistant superbugs

    Zengchao GuoWeiwei LiuTengfei LiuJinpeng Wang...
    319-324页
    查看更多>>摘要：With the increasing emergence of bacterial infections,especially multidrug-resistant(MDR)bacteria,poses an urgent threat.This study demonstrated a novel multifunctional nanotheranostics platform de-veloped by the strategic integration of both in-situ bio-assembly imaging and target bacteria inacti-vation.Through the introduction of copper ions into bacteria,the Cu2+could spontaneously bio-self-assembled into a multifunctional copper nanoclusters(NCs)which efficiently enhanced epigallocatechin gallate(EGCG)uptake into bacteria.While visualizing the bacteria,the developed theranostic nanoplat-form exhibited highly efficient disinfection activities with negligible side effects as reflected by higher cell viability and insignificant hemolytic effects.Furthermore,the exosomal formulation of EGCG inte-grated with Cu2+showed an increased intracellular antibacterial activity,which could eliminate most of the methicillin-resistant Staphylococcus aureus(MRSA)phagocytosed by macrophages,guide macrophages toward M2-like phenotype polarization and alleviate inflammation,without exhibiting obvious cytotox-icity on host RAW264.7.The regimen could be viewed as an effective strategy for the sterilization of intractable bacterial infections.
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    FRET-based two-photon benzo[a]phenothiazinium photosensitizer for fluorescence imaging-guided photodynamic therapy

    Yiling LiZekun GaoXiuxiu YueMinhuan Lan...
    325-328页
    查看更多>>摘要：To overcome the conflict between the long-wavelength excitation and high singlet oxygen quantum yield of photosensitizers,we conjugated a two-photon fluorophore,tetrahydroquinoxaline coumarin(TQ),and an efficient photodynamic therapeutic agent,benzo[a]phenothiazinium(NBS-NH2),through a hexamethy-lene linker to build a two-photon photosensitizer,TQ-NBS.In TQ-NBS,TQ served as an energy donor and NBS-NH2 acted as an energy acceptor;and TQ-NBS was a Förster resonance energy transfer(FRET)cas-sette with a 92.8% efficiency.The large two-photon absorption cross-section of TQ allowed photosensitizer TQ-NBS to work in a 900nm two-photon excitation(TPE)mode,which greatly benefited the deep tissue penetration in PDT treatment.Meanwhile,the excellent phototoxicity and near-infrared fluorescence of NBS-NH2 was kept in TQ-NBS under a TPE mode via a FRET process.Photosensitizer TQ-NBS exhibited a high phototoxic efficacy in living cells and tumor-bearing mice.
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    Pairs of thiol-substituted 1,2,4-triazole-based isomeric covalent inhibitors with tunable reactivity and selectivity

    Shiqi XuZi YeShuang ShangFengge Wang...
    329-335页
    查看更多>>摘要：Covalent bioactive compounds are successfully used in clinic and attracted intense research efforts in the fundamental study as well as drug development.The advantageous effects of covalent compounds compared with non-covalent ones are highly dependent on electrophilic warheads.Hence,electrophilic warheads with tunable reactivity and selectivity are highly demanded in fields of medicinal chemistry and chemical biology.Herein,we report a novel electrophilic warhead,chloromethyl group activated by thiol-substituted 1,2,4-triazole.Interestingly,a pair of regioisomers could be simultaneously occurred in the step of alkylation during the synthesis of this unique motif.This is a rare example that the alkyla-tion could simultaneously generate these two separable regioisomers of 1,2,4-triazole at the nitrogen or sulfur atom.The covalent-working mechanism of this new warhead is confirmed by various chemopro-teomics experiments including target identification and binding site mapping.Importantly,the reactivity and selectivity of this new electrophilic warhead could be efficiently tuned by virtue of stereo effect.In-terestingly,one pair of regioisomers(19S and 19X)induced distinct modes of cell death.Isomer 19S could induce apoptosis of colon cancer cells while 19X could induce both apoptosis and ferroptosis.Together,this study provides pairs of novel electrophilic warheads that could be useful not only in supporting the design of covalent compounds for drug discovery but also in providing chemical probes for the funda-mental biological study.
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    Controlling molecular assembly on time scale:Time-dependent multicolor fluorescence for information encryption

    Zixi ZouJingyuan WangYian SunQian Wang...
    336-340页
    查看更多>>摘要：Dynamic assembly on time scale is common in biological systems but rare for artificial materials,espe-cially for smart luminescent materials.Programming molecular assembly in a spatio-temporal manner and resulting in white-light-including multicolor fluorescence with time-dynamic features remains chal-lenging.Herein,controlling molecular assembly on time scale is achieved by integrating a pH-responsive motif to a transient alkaline solution which is fabricated by activators(NaOH)and deactivators(esters),leading to automatic assembly on time scale and time-dependent multicolor fluorescence changing from blue to white and yellow.The kinetics of the assembly process is dependent on the ester hydrolysis process,which can be controlled by varying ester concentrations,temperature,initial pH,stirring rate and ester structures.This dynamic fluorescent system can be further developed for intelligent fluores-cent materials such as fluorescent ink,three-dimension(3D)codes and even four-dimension(4D)codes,exhibiting a promising potential for information encryption.
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    Pyridapeptides F-I,cyclohexapeptides from marine sponge-derived Streptomyces sp.OUCMDZ-4539

    Shuige ZhaoPengcheng YanPeipei LiuHaishan Liu...
    341-344页
    查看更多>>摘要：Four new cyclohexapeptides,pyridapeptides F-I(1-4),were isolated from the fermentation broth of marine sponge-derived Streptomyces sp.OUCMDZ-4539.The pyridapeptides F-H(1-3)are com-posed of β-hydroxyleucine,alanine,O-methylthreonine,hexahydropyridazine-3-carboxylic acid,5-hydroxytetrahydropyridazine-3-carboxylic acid,and(2S,3R,4E,6E)-2-amino-3-hydroxy-4,6-dienoic acid residues.Pyridapeptide I(4)contains(2S,3R,4E,6E)-2-amino-3-hydroxy-8-methylnona-4,6-dienoic acid residue and a very rare glycose residue,aculose.Their structures were determined based on spectroscopic analysis and chemical methods.Pyridapeptides G-I(2-4)have the 2,3,6-trideoxyhexose units glycosy-lated at the γ-OH-TPDA residue,displayed significant antiproliferative activity against four(PC9,MKN45,HepG2,K562)or two(PC9,MKN45)human cancer cell lines.
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    Genome mining of multi-substituted alkylresorcinols from a hybrid highly reducing-and type Ⅲ-polyketide pathway

    Huaran ZhangYuting HuangYingjie TangDekun Kong...
    345-349页
    查看更多>>摘要：Fungal alkylresorcinols are a class of polyketides,which are commonly synthesized by the hybridization of highly reducing polyketide synthase(hrPKS)with non-reducing polyketide synthase(nrPKS).In this study,we identified and demonstrated a new assembly model for synthesizing alkylresorcinol(scirpilin A,1),which was accomplished by collaboration of a hrPKS(FscA)and a type Ⅲ PKS(FscB).Furthermore,three post-tailoring enzymes(FscC,FscD,and FscE)act iteratively on 1 skeleton,including successive 14e-oxidation of inert carbons,di-halogenation,and di-methylation,to form highly oxidized and multi-substituted alkylresorcinols.Our work presents an unusual synthesis manner of alkylresorcinols,sheds light on the collaborative mechanism between hrPKS and type Ⅲ PKS and provides three valuable enzy-matic catalysts for the tailoring of alkylresorcinol family natural products in future.
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    Phomaketals A and B,pentacyclic meroterpenoids from a eupC overexpressed mutant strain of Phoma sp.

    Chuan LiYangyang HanYanan ZhaiKe Li...
    350-354页
    查看更多>>摘要：Phomaketals A(1)and B(2),two tropolonic meroterpenoids with the unprecedented pentacyclic skele-tons,were isolated from the solid-substrate fermentation cultures of a eupC overexpressed mutant strain of the fungus Phoma sp.,together with a biogenetically related secondary metabolite pughiinin B(3),and the known one noreupenifeldin B(4).The structures of 1-3 were elucidated primarily by nuclear magnetic resonance(NMR)experiments.The absolute configurations of 1 and 2 were assigned by elec-tronic circular dichroism calculations and the calculated NMR with DP4+analysis,while that of 3 was established by single-crystal X-ray diffraction analysis using Cu Kα radiation.Biogenetically,phomaketals A(1)and B(2)could be derived from the hypothetical tropolonic sesquiterpene intermediates neose-tophomone B(6)and 9-R-neosetophomone B(6′),respectively,via different reactions cascades.Com-pound 1 showed antiproliferative effect only against the SUPB15 cells,with an 50% inhibitory concentra-tion(IC50)value of 4.85μmol/L,while the co-isolated known meroterpenoid 4 displayed potent effects against three tumor cell lines,SUPB15,EL4,and H9,showing IC50 values of 0.36-27.08 μmol/L.
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