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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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    Continuous-flow synthesis of polysubstituted γ-butyrolactones via enzymatic cascade catalysis

    Liliang ChuXiaoyan ZhangJianing LiXuelei Deng...
    404-408页
    查看更多>>摘要：Polysubstituted chiral γ-butyrolactones are the core structural units of many natural products and high value-added flavors and fragrances used in the food and cosmetic industry.Current enzymatic cascade synthesis of these molecules faces the problems of low enzyme activity and phase separation in batch reaction,resulting in low productivity.Herein,we report a new continuous-flow process to synthesize the optically pure Nicotiana tabacum lactone(3S,4S)-4a and whisky lactone(3R,4S)-4b from α,β-unsaturatedγ-ketoesters.A new ene reductase(ER)from Swingsia samuiensi(SsER)and a carbonyl reductase(SsCR)were engineered by directed evolution to improve their activity and thermostability.The continuous-flow preparative reactions were performed in two 3D microfluidic reactors,generating(3S,4S)-4a(99％ee and 87％de)and(3R,4S)-4b(99％ee and 98％de)with space-time yields 3 and 7.4 times higher than those of the batch reactions.The significant enhancement in the productivity of enzyme cascade catalysis brought by cutting-edge continuous microfluidic technology will benefit the general multi-enzyme catalytic sys-tems in the future.
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    Carbon dot-based artificial light-harvesting systems with sequential energy transfer and white light emission for photocatalysis

    Chaoqun MaYuebo WangNing HanRongzhen Zhang...
    409-413页
    查看更多>>摘要：In this work,we designed and synthesized cationic carbon dots(CDs)with a size distribution of 1.6-3.7 nm,which exhibited dark blue fluorescence in the aqueous solution.Based on its excellent lumi-nescence properties,we used it as an energy donor to construct a sequential artificial light-harvesting system(LHS)by employing the energy-matching dyes eosin Y disodium salt(EY)and sulforhodamine 101(SR101),which could regulate the white light emission(Commission Internationale de l'Eclairage(CIE)coordinate:(0.30,0.31))with the energy transfer efficiency(ΦET)of 53.9％and 20.0％.Moreover,a single-step artificial LHS with white light emission(0.32,0.28)can be constructed directly using CDs and dye solvent 43(SR)with ΦET and antenna effect(AE)of 48.8％and 6.5,respectively.More importantly,CDs-based artificial LHSs were firstly used in photocatalytic of α-bromoacetophenone,with a yield of 90％.This work not only provides a new strategy for constructing CDs-based LHSs,but also opens up a new application for further applying the energy harvested in CDs-based LHSs to the field of the aqueous solution photocatalysis.
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    Bi-doped carbon quantum dots functionalized liposomes with fluorescence visualization imaging for tumor diagnosis and treatment

    Peide ZhuYangjia LiuYaoyao TangSiqi Zhu...
    414-419页
    查看更多>>摘要：Liposomes are one of the significant classes of antitumor nanomaterials and the most successful nanomedicine drugs in clinical translation.However,it is difficult to accurately reveal liposome deliv-ery modes and drug release rates at different pH values to assess the biodistribution and drug deliv-ery pathways in vivo.Here,we established a strategy to integrate Bi-doped carbon quantum dots(CQDs)with liposomes to produce fluorescence visualization and therapeutic effects,namely lipo/Bi-doped CQDs.Lipo/Bi-doped CQDs show good water solubility and physicochemical properties,which can be used for in vitro labeling of colon cancer(CT26)cells and in vivo imaging localization tracking tumors for mon-itoring.Simultaneously,thanks to the excellent pH sensitivity and ion doping characteristic of Bi-doped CQDs,lipo/Bi-doped CQDs can be used to reveal the drug release rate of liposomes at different pH values and exhibit potential effects in vivo antitumor therapy.
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    Lysosome-targeted carbon dots with a light-controlled nitric oxide releasing property for enhanced photodynamic therapy

    Hao CaiXiaoyan WuLei JiangFeng Yu...
    420-425页
    查看更多>>摘要：The reactive oxygen species(ROS)generation efficiency is always limited by the extreme tumor mi-croenvironment(TME),leading to unsatisfactory antitumor effects in photodynamic therapy(PDT).As a promising gas therapy molecule,nitric oxide(NO)is independent of oxygen and could even synergize ROS to enhance the therapeutic effect.However,the short half-life,instability,and uncontrollable release of exogenous NO limited the application of tumor synergistic therapy.Herein,we reported a novel kind of red-emissive carbon dots(CDs)that was capable of lysosome-targeted and light-controlled NO deliv-ery.The CDs were synthesized by using metformin and methylene blue(MB)via a hydrothermal method.The obtained metformin-MB CDs(MMCDs)exhibited a higher 1O2 quantum yield and NO generation efficiency under light emitting diode(LED)light irradiation.Noteworthily,the 1O2 could further in situ oxidize NO into peroxynitrite anions(ONOO-),which own the higher cytotoxicity against cancer cells.Cell experiments indicate that MMCDs could destruct lysosome membrane integrity and kill almost 80％of HepG2 cells under light irradiation while very low cytotoxicity in the dark.Moreover,MMCDs signif-icantly decreased tumor volume and weight after phototherapy in hepatoma HepG2-bearing mice.Our study provides a new strategy for light-controlled NO generation as well as precise lysosome-targeting for enhancement of PDT efficiency.
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    A novel insight of enhancing the hydrogen peroxide tolerance of unspecific peroxygenase from Daldinia caldariorum based on structure

    Tiantian LiRuochen JinBin WuDongming Lan...
    426-430页
    查看更多>>摘要：Unspecific peroxygenases(UPOs,EC 1.11.2.1)is a kind of thioheme enzyme capable of catalyzing various oxidations of inert C-H bonds using H2O2 as an oxygen donor without cofactors.However,the enhance-ment of the H2O2 tolerance of UPOs is always challenging.In this study,the A161C mutant of rDcaUPO,which originates from Daldinia caldariorum,was found to be highly H2O2-resistant.Compared with the wild type,the mutant rDcaUPO-A161C showed a 10-h prolonged half-life and a 64％improved enzyme ac-tivity when incubated in 10mmol/L H2O2.The crystal structure analysis at 1.47 Å showed that rDcaUPO-A161C exhibited 10 α-helixes(cyan)and a series of ordered rings,forming a single asymmetric spherical structure.The two conserved domains near heme formed an active site with the catalytic PCP and EHD regions(Glu86,His87,Asp88 residues).The H2O2 tolerance of rDcaUPO-A161C was preliminarily explored by comparing its structure with the wild type.Notably,rDcaUPO-A161C showed significantly higher cat-alytic efficiency than the wild type for the production of hydroxyl fatty acids.This study is anticipated to provide an insight into the structure-function relationship and expand potential applications of UPOs.
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    Polyethylene interfacial dielectric layer for organic semiconductor single crystal based field-effect transistors

    Min ChenBoyu PengXuyun GuoYe Zhu...
    431-435页
    查看更多>>摘要：Organic semiconductor single crystals(OSSCs)have shown their promising potential in high-performance organic field-effect transistors(OFETs).The interfacial dielectric layers are critical in these OFETs as they not only govern the key semiconductor/dielectric interface quality but also determine the growth of OSSCs by their wetting properties.However,reported interfacial dielectric layers either need rig-orous preparation processes,rely on certain surface chemistry reactions,or exhibit poor solvent re-sistance,which limits their applications in low-cost,large-area,monolithic fabrication of OSSC-based OFETs.In this work,polyethylene(PE)thin films and lamellar single crystals are utilized as the inter-facial dielectric layers,providing solvent resistive but wettable surfaces that facilitate the crystallization of 6,13-bis(tri-isopropylsilylethynyl)pentacene(TIPS-PEN)and 6,13-bis(triisopropylsilylethynyl)-5,7,12,14-tetraazapentacene(TIPS-TAP).As evidenced by the presence of ambipolar behavior in TIPS-PEN single crystals and the high electron mobility(2.3±0.34 cm2 V-1 s-1)in TIPS-TAP single crystals,a general im-provement on electron transport with PE interfacial dielectric layers is revealed,which likely associates with the chemically inertness of the saturated C-H bonds.With the advantages in both processing and device operation,the PE interfacial dielectric layer potentially offers a monolithic way for the enhance-ment of electron transport in solution-processed OSSC-based OFETs.
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    Near-infrared non-fused electron acceptors for efficient organic photovoltaics

    Wenxiang MaXinyu HeTianyi ChenDe-Li Ma...
    436-441页
    查看更多>>摘要：Developing narrow-bandgap organic semiconductors is important to facilitate the advancement of or-ganic photovoltaics(OPVs).Herein,two near-infrared non-fused ring acceptors(NIR NFRAs),PTBFTT-F and PTBFTT-Cl have been developed with A-πA-π D-D-πD-πA-A non-fused structures.It is revealed that the introduction of electron deficient π-bridge(πA)and multiple intramolecular noncovalent interac-tions effectively retained the structural planarity and intramolecular charge transfer of NFRAs,extending strong NIR photon absorption up to 950 nm.Further,the chlorinated acceptor,with the enlarged π-surface compared to the fluorinated counterpart,promoted not only molecular stacking in solid,but also the desirable photochemical stability in ambient,which are helpful to thereby improve the exciton and charge dynamics for the corresponding OPVs.Overall,this work provides valuable insights into the design of NIR organic semiconductors.
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    Trifluoromethyl enable high-performance single-emitter white organic light-emitting devices based on quinazoline acceptor

    Xiangan SongShaogang ShenMengyao LuYing Wang...
    442-446页
    查看更多>>摘要：Single-emitter white organic light-emitting diode(WOLED)based on small organic molecule exhibits great potential in simplifying fabrication process of WOLEDs.However,the design and synthesis of molecule for highly efficient single-emitter WOLED still remains a challenge.Herein,two asymmetric donor-acceptor-acceptor'(D-A-A')type molecule(PTZ-PQ-F and PTZ-PQ-CF3)are developed by employing trifluoromethyl(CF3)or fluorine atom as secondary acceptor,which can exhibit white lighting with dual emission bands consisting of blue traditional fluorescence from quasi-axial(ax)conformer and orange thermally activated delayed fluorescence(TADF)from quasi-equatorial(eq)conformer.The introduction of CF3 into PTZ-PQ-CF3 greatly enhanced the photoluminescence quantum yield(PLQY)by suppressing the nonradiative deactivation.Owing to electron-inductive-effect of CF3,the"eq"conformer of PTZ-PQ-CF3 exhibits a much smaller ΔEST of 0.01 eV to realize more efficient reverse intersystem crossing(RISC)process,and then enhance the exciton utilization(nearly 100％)of the whole dual emission system.Con-sequently,single-emitter WOLEDs based on PTZ-PQ-CF3 show nearly standard white emission with EQE of 13.0％and CIE of(0.35,0.36)in mCP host and show warm white emission with high EQE of 25.5％and CIE of(0.40,0.47)in 35 DczPPy host,which are the best performance among reported single-emitter WOLEDs.
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    Electron-transporting boron-doped polycyclic aromatic hydrocarbons:Facile synthesis and heteroatom doping positions-modulated optoelectronic properties

    Tingting HuangZhuanlong DingHao LiuPing-An Chen...
    447-451页
    查看更多>>摘要：While heteroatom doping serves as a powerful strategy for devising novel polycyclic aromatic hydro-carbons(PAHs),the further fine-tuning of optoelectronic properties via the precisely altering of doping patterns remains a challenge.Herein,by changing the doping positions of heteroatoms in a diindenopy-rene skeleton,we report two isomeric boron,sulfur-embedded PAHs,named Anti-B2S2 and Syn-B2S2,as electron transporting semiconductors.Detailed structure-property relationship studies revealed that the varied heteroatom positions not only change their physicochemical properties,but also largely affect their solid-state packing modes and Lewis base-triggered photophysical responses.With their low-lying fron-tier molecular orbital levels,n-type characteristics with electron mobilities up to 1.5 × 10-3 cm2 V-1 s-1 were achieved in solution-processed organic field-effect transistors.Our work revealed the critical role of controlling heteroatom doping patterns for designing advanced PAHs.
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    Near-infrared double-cable conjugated polymers based on alkyl linkers with tunable length for single-component organic solar cells

    Yikun WangQiaomei ChenShijie LiangDongdong Xia...
    452-456页
    查看更多>>摘要：The photovoltaic properties of double-cable conjugated polymers are significantly influenced by the length of the alkyl linkers that connect donor backbones and acceptor side units.In this study,a series of 2-(3-oxo-2,3-dihydroinden-1-ylidene)malononitrile(IC)-based double-cable polymers with alkyl linkers ranging from C8H16 to C16H32(Px,x=8,10,12,14,16)were synthesized for single-component organic solar cells(SCOSCs).Among these,the linker length x=12(P12)is found to optimize the power conver-sion efficiencies(PCEs)in SCOSCs.Specifically,PCEs increase from P8 to P12 and then decline from P12 to P16.Detailed investigations of optical absorption,charge transport,and morphology provide insights into the underlying factors contributing to these PCE variations.The findings indicate that the excep-tional photovoltaic properties observed in P12 can be attributed to three key factors:A delicate balance between enhanced charge separation facilitated by the increased spacer length and reduced crystallinity resulting from longer spacers,higher charge mobilities,and well-balanced hole/electron transport charac-teristics.This study highlights the critical role of linker length in determining the photovoltaic properties of double-cable conjugated polymer-based SCOSCs and offers valuable guidance for the design of novel double-cable conjugated polymers.
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