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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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    A fungal CYP from Beauveria bassiana with promiscuous steroid hydroxylation capabilities

    Yu PengYue WangTian-Jiao ChenJing-Jing Chen...
    218-222页
    查看更多>>摘要：Hydroxylation of steroid core is critical to the synthesis of steroid drugs.Direct sp3 C-H hydroxylation is challenging through chemical catalysis,alternatively,fungal biotransformation offers a possible solu-tion to this problem.However,mining and metabolic engineering of cytochrome P450 monooxygenases(CYPs)is usually regarded as a more eco-friendly and efficient strategy.Herein,we report the mining and identification of a new steroid CYP(CYP68BE1)from Beauveria bassiana by transcriptomics,heterologous expression,in vivo and in vitro functional characterization.The catalytic promiscuity of CYP68BE1 was explored,and CYP68BE1 showed promiscuously and catalytically versatile,which is qualified for mono-hydroxylation on C11α,C1α,C6β and dihydroxylation on C1β,11α and C6β,11α of six steroids,leading to the production of key steroid intermediates required in the industrial synthesis of some indispensable steroid drugs.Molecular dynamics simulations were performed,revealing the molecular basis of different binding orientations of CYP68BE1 with different substrates.The discovery of CYP68BE1 offers a promis-ing biocatalyst for enriching the steroid structural and functional diversity,which also can be applied to biosynthesize valuable steroid drug intermediates.
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    Effective assignment of positional isomers in dimeric shikonin and its analogs by 1H NMR spectroscopy

    Ling-Hao ZhaoHai-Wei YanJian-Shuang JiangXu Zhang...
    223-226页
    查看更多>>摘要：An approach for distinguishing two types of positional isomers of dimeric shikonin and its analogs was explored with 4JC,H long-range correlation by prolonging the acquisition time at 2,3Jc,H values of 2.0 and 8.0 Hz.Furthermore,the 1H(proton)nuclear magnetic resonance(NMR)pattern of phenolic hydroxyl protons was developed as a"diagnosis signal"to ascertain the relative location of each side chain in DMSO-d6 at sample concentrations of 0.022-0.034 mol/L.The chemical shift differences of 0.6 ppm be-tween OH-5'and OH-1 and between OH-8'and OH-4 are assigned to Type A and Type B,respectively.All reported ambiguous structures were corrected by this pattern.Additionally,the steric structures of isolated compounds were elucidated by quantum chemical calculations of electronic circular dichroism(ECD)spectra.
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    Electron push-pull effects induced performance promotion in covalent organic polymer thin films-based memristor for neuromorphic application

    Panke ZhouHong YuMun Yin CheeTao Zeng...
    227-231页
    查看更多>>摘要：Covalent organic polymer(COP)thin film-based memristors have generated intensive research interest,but the studies are still in their infancy.Herein,by controlling the content of hydroxyl groups in the aldehyde monomer,Py-COP thin films with different electronic push-pull effects were fabricated bearing distinct memory performances,where the films were prepared by the solid-liquid interface method on the ITO substrates and further fabricated as memory devices with ITO/Py-COPs/Ag architectures.The Py-COP-1-based memory device only exhibited binary memory behavior with an ON/OFF ratio of 1∶101.87.In contrast,the device based on Py-COP-2 demonstrated ternary memory behavior with an ON/OFF ratio of 1∶100.6∶103.1 and a ternary yield of 55％.The ternary memory mechanism of the ITO/Py-COP-2/Ag memory device is most likely due to the combination of the trapping of charge carriers and conductive filaments.Interestingly,the Py-COPs-based devices can successfully emulate the synaptic potentiation/depression behavior,clarifying the programmability of these devices in neuromorphic systems.These results suggest that the electronic properties of COPs can be precisely tuned at the molecular level,which provides a promising route for designing multi-level memory devices.
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    Carbon dots-enhanced pH-responsive lubricating hydrogel based on reversible dynamic covalent bondings

    Jianye KangXinyu YangXuhao YangJiahui Sun...
    232-237页
    查看更多>>摘要：Due to the various pH liquid environment in nature,the pH-responsive lubricating hydrogel is widely investigated and developed for tissue interface substitute.However,the applied liquid environment will lead to poor mechanical property and weaken the pH-responsive capability.In this work,a carbon dots-enhanced pH-responsive lubricating hydrogel is developed by combining a pH-responsive section of dy-namic PVA-borax network into a PAAm covalent polymer network.The formed hydrogel presents a par-tial gel-sol transition under controlled pH environments.At low pH environments(＜6.0),the formed lubricating layer originated from dynamic disassembly of PVA-borax hydrogel,and brings the lubricating properties on the hydrogel surface.Moreover,the mechanical strength and lubrication properties are well promoted by introducing the carbon dots into the hydrogel,the blue sol layer can be observed more vi-sually under the fluorescence microscope.The pH-response also exhibits well reversibility.The prepared hydrogel broadens the idea for designing pH-responsive soft materials for soft lubricating actuator or robot.
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    A weak but inert hindered urethane bond for high-performance dynamic polyurethane polymers

    Fangzhou WangWentong GaoChenghui Li
    238-243页
    查看更多>>摘要：Covalent adaptable networks(CANs),which share the properties of both thermosets and thermoplastics at the same time,are desirable for many applications.Introducing bulky substituents is a feasible way to design dynamic covalent bonds for constructing CANs,as evidenced by the successful implementa-tion in CANs based on hindered urea bonds(HUBs).However,the dynamicity induced by introducing bulky substituents always come with low bond energy,resulting in low mechanical strength and poor stability of the CANs.Herein,we designed a novel hindered urethane bond,which is weak in thermody-namic(Keq=1701.23 L/mol at 25 ℃)and inert in kinetic at low temperature,but stable in thermodynamic(Keq=1.54 × 104L/mol at 100 ℃)and active in kinetic at high temperature(k-1=0.105 h-1 at 80 ℃ and 0.315 h-1 at 120 ℃).As a result,the polyurethane based on it exhibits high mechanical properties(with Youngs'modulus of 1011±29 MPa and flexible modulus reached 1833±50 MPa)and excellent reversibil-ity(can be reprocessed at 60 ℃ under 100 kPa in 30 min and completely healed at 40 ℃ in 10 min).Moreover,unlike to many CANs based on hindered urea bonds,our dynamic polyurethanes are highly stable in humid environment or even water solutions due to the slow hydrolysis kinetics.Such high-performance dynamic polyurethane polymers are attractive for many applications.
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    Nonalternant isomer of pentacene fusing two azulene units

    Bo YuPengchen DuJianwen GuoHanshen Xin...
    244-248页
    查看更多>>摘要：Azulene is a promising building block for creating innovative polycyclic aromatic hydrocarbons.This study involved the construction of three nonalternant isomers of pentacene by fusing two azulene units,named Az-PH1/2/3.Az-PH1 was initially developed through the rhodium(Ⅱ)-catalyzed cyclization of bis(N-tosylhydrazone)s.Intriguingly,Az-PH1 was also unexpectedly obtained during a nickel(0)-catalyzed one-step tandem reaction.We investigated the optical and electrochemical properties,aromaticity,and photo-oxidative stability of Az-PH1,comparing it with the well-known pentacene using density functional theory,electrochemical,and photophysical tests.Our results showed that the azulene-fusing strategy re-sulted in a molecule with narrow optical bandgaps(2.046 eV)and a long half-life time under ambient air conditions.
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    Thienothiophene-centered ladder-type π-systems that feature distinct quinoidal π-extension

    Jiaxiang GuoZeyi LiTianyu ZhangXinyu Tian...
    249-253页
    查看更多>>摘要：Quinoidal π-conjugated structures,a kind of fundamental subunits for organic π-systems,may produce some intriguing optical,electronic and magnetic properties of polycyclic hydrocarbons(PHs).Herein,we report two thienothiophene-centered ladder-type polycyclic molecules(1 and 2),which possess one quinoidal thienothiophene moiety and two para-quinodimethane(p-QDM)subunits,respectively.As theoretically and experimentally studied,while 1 is a fully closed-shell molecule,2 owns an open-shell structure along with partial contribution of tetraradical state that is induced by the resonance of p-QDM.Moreover,although 2 has a larger π-conjugated skeleton and open-shell electronic state,it exhibits larger bandgap and blue-shifted absorption.On the other hand,the reversible oxidation activity of 1 enables the preparation of its dication 12+,and the studies on its single-crystal and aromatic structures demonstrate that its two positive charges are delocalized onto the oxygen atoms,thus achieving fullyπ-extended structure and near-infrared absorption.This study not only gains insight into quinoidal 7r-subunits,but also provides an important basis for the development of antiaromatic and open-shellπ-electron materials.
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    A simple photochemical method for surface fluorination using perfluoroketones

    Zhiwei ZhongYanbin HuangWantai Yang
    254-258页
    查看更多>>摘要：Surface fluorination of conventional polymers can give them desirable surface properties similar to the expensive and difficult-to-process fluoropolymers.However,traditional surface fluorination tech-niques often require toxic reagents and special equipment.Here,we report a simple and effective poly-mer surface fluorination method by using safe and inexpensive perfluoro-2-methyl-3-pentanone(PFMP,C2F5C(=O)CF(CF3)2)and UV irradiation.This method is applicable to various polymer materials,and gen-erates nanometer-thick fluorinated layer on the outermost surface,significantly changing their surface properties without changing the surface morphology.
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    Sequence design in terpolymerization of ε-caprolactone,CO2 and cyclohexane oxide:Random ester-carbonate distributions lead to large-span tunability

    Zhenjie YangChenyang HuXuan PangXuesi Chen...
    259-264页
    查看更多>>摘要：It is of great interest to make a degradable material widely tailorable to replace petroleum-derived prod-ucts among diverse applications.Here,we report the construction of a new multi-purpose degradable material for the first time via a simple ternary copolymerization system comprising ε-caprolactone(ε-CL),cyclohexane oxide(CHO)and CO2.Under low pressure of 1 bar～5 bar,the ring-opening polymerization(ROP)of ε-CL and ring-opening copolymerization(ROCOP)of CO2 and CHO can simultaneously proceed.The carbonate units are randomly distributed on the polymer chain.These random terpolymers have con-trollable molar mass(10-106kDa)and compositions(4-33 mol％CO2).And the obtained materials show large-span tunability from tough plastic to elastomer and even adhesive.
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    Improving the electrocatalytic performances of Pt-based catalysts for oxygen reduction reaction via strong interactions with single-CoN4-rich carbon support

    Jin LongXingqun ZhengBin WangChenzhong Wu...
    265-271页
    查看更多>>摘要：Developing platinum-group-metal(PGM)catalysts possessing strong metal-support interaction and con-trollable PGM size is urgent for the sluggish oxygen reduction reaction(ORR)in proton-exchange mem-brane fuel cells.Herein,we propose an in-situ self-assembled reduction strategy to successfully induce highly-dispersed sub-3nm platinum nanoparticles(Pt NPs)to attach on resin-derived atomic Co coordi-nated by N-doped carbon substrate(Pt/CoSA-N-C)for ORR.To be specific,the interfacial electron inter-action effect,along with a highly robust CoSA-N-C support endow the as-fabricated Pt/CoSA-N-C catalyst with significantly enhanced catalytic properties,i.e.,a mass activity(MA)of 0.719 A/mgPt at 0.9 ViR-free and a reduction of 24.2％in MA after a 20,000-cycles test.Density functional theory(DFT)calculations demonstrate that the enhanced electron interaction between Pt and CoSA-N-C support decreases the d-band center of Pt,which is in favor of lowering the desorption energy of*OH on Pt/CosA-N-C surface and accelerating the formation of H2O,thus enhance the instinct activity of ORR.Furthermore,the higher binding energy between Pt and CoSA-N-C compared to Pt and C indicates that the migration of Pt has been suppressed,which theoretically explains the improved durability of Pt/CoSA-N-C.Our work offers an enlightenment on constructing composite Pt-based catalysts with multiple active sites.
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