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中国化学（英文版）
科学出版社
中国化学（英文版）

科学出版社

月刊

1001-604X

上海市枫林路354号

中国化学（英文版）/Journal Chinese Journal of ChemistryCSCDCSTPCD北大核心SCI
查看更多>>本刊系中国科协主管、中国化学会、中国科学院上海有机化学研究所主办。刊载物理化学、无机化学、有机化学和分析化学等各学科领域基础研究和应用基础研究的原始性研究成果。
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    Identification of in situ Generated Iron-Vacancy Induced Oxygen Evolution Reaction Kinetics on Cobalt Iron Oxyhydroxide

    Na YaoJuan ZhuHongnan JiaHengjiang Cong...
    343-350页
    查看更多>>摘要：Developing highly efficient and low-cost electrocatalysts towards oxygen evolution reaction(OER)is essential for practical applica-tion in water electrolyzers and rechargeable metal-air batteries.Although Fe-based oxyhydroxides are regarded as state-of-the-art non-noble OER electrocatalysts,the origin of performance enhancement derived from Fe doping remains a hot topic of considerable discussion.Herein,we demonstrate that in situ generated Fe vacancies in the pristine CoFeOOH catalyst through a pre-conversion process during alkaline OER result from dynamic Fe dissolution,identifying the origin of Fe-vacancy-induced enhanced OER kinetics.Density functional theory(DFT)calculations and experimental results including X-ray absorption fine-structure spectroscopy,in situ UV-Vis spectroscopy,and in situ Raman spectroscopy reveal that the Fe vacancies could significantly promote the d-band center and valence states of adjacent Co sites,alter the active site from Fe atom to Co atom,accelerate the formation of high-valent active Co4+species,and reduce the energy barrier of the potential-determining step,thereby contribute to the significantly enhanced OER per-formance.
      原文链接:
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    • 维普

    Decarboxylative Amination with Nitroarenes via Synergistic Catalysis

    Meiling DingSitian ZhouShunruo YaoChengjian Zhu...
    351-355页
    查看更多>>摘要：In this paper,we have developed a decarboxylative amination of carboxylic acids with nitroarenes for the synthesis of secondary amines.The protocol is performed at mild conditions without the use of noble metals as catalysts.A wide range of structurally diverse secondary amines could be obtained in good yields(up to 94％)with good functional group tolerance.This transformation shows good to excellent selectivity,avoiding the generation of over alkylated byproducts.
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    Nickel-Catalyzed Stereoselective Migratory Carboboration of 1,4-Cyclohexadiene

    Yaoyu RenLujin WangChao DingYangyang Li...
    356-362页
    查看更多>>摘要：Multi-substituted cyclohexanes play a crucial role as scaffolds in bioactive compounds.While significant progress has been made in synthesizing substituted cyclohexanes,methods for the stereoselective assembly of 1,3-disubstituted cyclohexanes remain scarce.This study presents a novel approach involving nickel catalysis to achieve stereoselective carboboration of 1,4-cyclohexadiene.This innova-tive process allows for the simultaneous introduction of a boron group and an aryl or an alkyl fragment into the 1,4-cyclohexadiene framework under mild conditions,with exclusive regioselectivity and excellent cis configuration.The resulting products feature a dou-ble carbon bond and the incorporation of the boron group,offering significant potential for subsequent transformations and down-stream applications.
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    Cobalt-Catalyzed Switchable[4+1]and[4+1+1]Spirocyclization of Aromatic Amides with 2-Diazo-1H-indene-1,3(2H)-dione:Access to Spiro Indene-2,1'-isoindolinones and Spiro lsochroman-3,1'-isoindolinones

    Bin LiMengmeng XieJingyu LiNana Shen...
    363-369页
    查看更多>>摘要：Herein,we report a condition-controlled divergent synthesis of spiro indene-2,1'-isoindolinones and spiro isochroman-3,1'-isoindoli-nones through cobalt-catalyzed formal[4+1]and[4+1+1]spirocyclization of aromatic amides with 2-diazo-1H-indene-1,3(2H)-dione.When the reaction is carried out under air in ethyl acetate,spiro indene-2,1'-isoindolinones are formed through Co(Ⅱ)-cata-lyzed C—H/N—H[4+1]spirocyclization.When the reaction is run under O2 in CH3CN,on the other hand,spiro isochroman-3,1'-iso-indolinones are generated through Baeyer-Villiger oxidation of the in situ formed spiro indene-2,1'-isoindolinones with O2 as a cheaper and environmental-friendly oxygen source.In general,these protocols have advantages such as using non-precious and earth-abundant metal catalyst,no extra additive,high efficiency and regioselectivity.A gram-scale synthesis and the removal of the directing group further highlight its utility.
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    Oxidative Dehydrogenation of Propane over Supported Nickel Single-Atom Cyatalyst

    Qian ZhangXunzhu JiangYangyang LiYuanlong Tan...
    370-376页
    查看更多>>摘要：Oxidative dehydrogenation of propane has been an ever-growing field for propylene production due to its exothermic properties,of which overoxidation is the major drawback,with CO and even CO2 as undesired by-products.For the purpose of getting higher pro-pylene selectivity as well as yield,herein,we report Ni single atoms supported on calcium aluminate as an efficient catalyst candidate for propane oxidative dehydrogenation.Beneficial from higher valence states of Ni1 species,it shows 2-3 times as much propylene selectivity as that of Ni nanoparticles.About 14.2％C3H6 yield with 47.3％propylene selectivity has been achieved on Ni single atom catalyst and a good stability during 20 h test can be obtained as well.
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    Manipulating Nanowires in Interconnecting Layer for Efficient Tandem Organic Photovoltaics

    Yanjie TangJiaming FuHao LiDu Hyeon Ryu...
    377-383页
    查看更多>>摘要：Owing to the function of manipulating light absorption distribution,tandem organic solar cells containing multiple sub-cells exhibit high power conversion efficiencies.However,there is a substantial challenge in precisely controlling the inter-subcells carrier migra-tion which determines the balance of charge transport across the entire device.The conductivity of"nanowires"-like conducting channel in interconnecting layer between sub-cells should be improved which calls for fine engineering on the morphology of poly-electrolyte in interconnecting layer.Here,we develop a simple method to effectively manipulating the domains of conductive com-ponents in commercially available polyelectrolyte PEDOT:PSS.The use of poor solvent could effectively modify the configuration of polystyrene sulfonic acid and thus the space for conductive components.Based on our strategy,the insulated shells wrapping con-ductive domains are thinned and the efficiencies of tandem organic solar cells are improved.We believe our method might provide guidance for the manufacture of tandem organic solar cells.
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    Establishing Modular Cell-Free Expression System for the Biosynthesis of Bicyclomycin from a Chemically Synthesized Cyclodipeptide

    Yi-Pei LiuYu-Heng ZhaoWen-Qi ZhangLian Wu...
    384-390页
    查看更多>>摘要：Cell-free expression systems have emerged as a versatile and powerful platform for metabolic engineering,biosynthesis and synthetic biology studies.Nevertheless,successful examples of the synthesis of complex natural products using this system are still limited.Bi-cyclomycin,a structurally unique and complex diketopiperazine alkaloid,is a clinically promising antibiotic that selectively inhibits the transcription termination factor Rho.Here,we established a modular cell-free expression system with cascade catalysis for the bio-synthesis of bicyclomycin from a chemically synthesized cyclodipeptide.The six cell-free expressed biosynthetic enzymes,including five iron-and α-ketoglutarate-dependent dioxygenases and one cytochrome P450 monooxygenase,were active in converting their substrates to the corresponding products.The co-expressed enzymes in the cell-free module were able to complete the related partial pathway.In vitro biosynthesis of bicyclomycin was also achieved by reconstituting the entire biosynthetic pathways(i.e.,six enzymes)using the modular cell-free expression system.This study demonstrates that the modular cell-free expression system can be used as a robust and promising platform for the biosynthesis of complex antibiotics.
      原文链接:
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    Strong Antiferromagnetic Exchange-Coupling Observed in Hydride-Bridged Dimeric Dysprosium(Ⅲ)Single-Molecule Magnet

    Qian-Cheng LuoKe-Xin YuPeng-Bo JinYe-Ye Liu...
    391-396页
    查看更多>>摘要：One dihydride-bridged dimeric Dy(Ⅲ)guanidinate complex,formulated as[{(Me3Si)2NC(NiPr)2}2Dy(μ-H)]2(1Dy),was successfully iso-lated and the introduction of hydride bridges significantly reduces the intramolecular Dy(Ⅲ)…Dy(Ⅲ)distance to only 3.688(1)Å.To in-vestigate the effect of such a short Dy(Ⅲ)…Dy(Ⅲ)distance on magnetism,we also prepared its dibromide-bridged analogue[{(Me3Si)2NC(NiPr)2}2Dy(μ-Br)]2(2Dy),which has a much longer Dy(Ⅲ)…Dy(Ⅲ)distance of 4.605(4)Å.Surprisingly,2Dy demonstrates much larger effective energy barrier for magnetization reversal(Ueff)and higher blocking temperature(TB).The worse performance of 1Dy is attributed to the concerted effect of strong antiferromagnetic interactions between Dy(Ⅲ)ions(Jtotal=-2.683 cm-1)and the unparallel arrangement of magnetic principle axes of the Dy(Ⅲ)ions for 1Dy.
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    Dual-Confined Bead-Like CoSe2@NC@NCNFs Bifunctional Catalyst Boosting Rechargeable Zinc-Air Batteries

    Kuixing DingJiugang HuLiming ZhaoHuanan Yu...
    397-405页
    查看更多>>摘要：Rationally developing efficient and durable bifunctional catalysts toward oxygen reduction reaction(ORR)and oxygen evolution re-action(OER)is critical for rechargeable zinc-air batteries(ZABs).Herein,a bead-like CoSe2@NC@NCNFs bifunctional catalyst was de-signed and fabricated by confining cubic CoSe2 nanoparticles to three-dimensional(3D)porous MOFs-derived nitrogen-doped car-bon(NC)and one-dimensional(1D)N-doped carbon nanofibers(NCNFs)through a facile encapsulate strategy.The 1D/3D continu-ous network structure contributes to the improvement of specific surface area and electronic conductivity,while the strong synergis-tic effect between CoSe2 sites and Co-Nx-C sites can effectively enhance electron/mass transfer and reduce the diffusion resistance.The as-constructed CoSe2@NC@NCNFs catalyst exhibits high catalytic activity and stability toward ORR/OER with a high half-wave potential of 0.80 V(vs.RHE)in ORR and a low overpotential of 280 mV at 10 mA·cm-2 in OER.More encouragingly,the rechargeable ZABs with CoSe2@NC@NCNFs cathode deliver high peak power densities(126.8 mW·cm-2),large specific capacities(763.1 mA·h·g-1),and robust charge-discharge cycling stability over 240 cycles.This study provides a facile strategy for designing efficient bifunctional catalysts for rechargeable energy conversion applications.
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    Recent Advances in Catalytic Carbonylation Reactions in Alternative Reaction Media

    Csaba árvaiLászló T.Mika
    406-429页
    查看更多>>摘要：Since the discovery of the hydroformylation(oxo-synthesis or Roelen reaction)and the Reppe-reaction,the transition metal-cata-lyzed carbonylation reactions,providing versatile,facile,and even atom-economic methods for the selective incorporation of C=O functionality to various skeletons,have gained tremendous importance in synthetic organic chemistry from laboratories to industrial applications.The carbonylation of carbon-carbon multiple bonds,aromatic halides,triflates,etc.,in the presence of various nucleo-philes has led the way to produce aldehydes,carboxylic acids,esters,amides,etc.,in the fine chemical industry.However,these protocols usually proceed in conventional,fossil-based,and usually toxic reaction environments.Thus,several attempts have been directed to developing efficient carbonylation methods in alternative,less harmful,non-fossil-based and even in renewable reaction media.In this review,we overview the recent applications of alternative solvents such as water,biomass-based alcohols,γ-valerolactone(GVL),2-methyltetrahydrofuran(2-MeTHF),ionic liquids(ILs),deep eutectic solvents(DES),alkyl levulinates,limo-nene,α-pinene,and dimethyl carbonate as well as fluorous media to improve efficiency,safety and environmentally benign nature of carbonylation protocols.
      原文链接:
    • 万方数据
    • 维普