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高等学校化学研究（英文版）
高等学校化学研究（英文版）

唐敖庆

双月刊

1005-9040

cjcu@mail.jlu.edu.cn

0431-88499216

130021

长春市解放大路117号吉林大学北区图书馆414室

高等学校化学研究（英文版）/Journal Chemical Research in Chinese UniversitiesCSCDCSTPCD北大核心SCI
查看更多>>本刊是中华人民共和国教育部委托吉林大学、南开大学主办的化学学科综合性学术刊物，以研究论文、研究快报、研究简报和综合评述等栏目集中报道我国高校和中科院研究所在化学学科及其交叉学科、新兴学科、边缘学科等领域所开展的基础研究，应用研究和重大开发研究所取得的最新成果。
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    Hierarchical Self-assembly of Atomically Precise Au Nanoclusters with Molecular Rotor-based Ligands

    WANG GuanzhongLU HuiLI JiangWANG Lihua...
    670-674页
    查看更多>>摘要：The hierarchical assemblies of precise nanoparticles(NPs)have created materials with emergent properties and functionalities.However,the complex assemblies remain unclear at a precise scale.Here,we show the hierarchical self-assembly of atomically precise gold nanoclusters(Au NCs)with molecular rotor-based ligands(MRL),featuring a double-layer surface.Compared to two other types of monolayer-protected(MLP)Au NCs,the significantly reduced surface density for MRL Au NCs profoundly influences their assembly behavior within the lattice.Furthermore the long length of rotor-based ligands and the rotational freedom of the phenyl-rings of rotor-based ligands also facilitate the assembly of NCs.Our works elucidate the hierarchical assembly on a precise scale,suggesting that the rotor-based ligand's strategy offers promising potential for designing well-defined and more complex structures in supercrystals.
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    A Scalable Pillar Layered Metal-Organic Framework for Natural Gas Purification

    LU NanLAN LanGAO QiangLI Na...
    675-681页
    查看更多>>摘要：One-step harvest of high-purity methane(CH4)from ternary propane/ethane/methane(C3H8/C2H6/CH4)mixtures remains a desirable yet challenging goal for natural gas purification.However,adsorbents either suffer from high capacity and selectivity,or are caught in a dilemma of scalable synthesis.Herein,we demonstrate a scalable pillar layered metal-organic framework Ni-MOF for highly efficient one-step CH4 purification.Ni-MOF exhibits high C2H6 and C3H8 uptakes of 83.3 and 86.1 cm3/g at 298 K and 100 kPa and remarkable C2H6/CH4(50/50,volume ratio,21.5)and C3H8/CH4(50/50,volume ratio,212.0)selectivities.Notably,high C2H6(42.2 cm3/g at 10 kPa)and C3H8(64.7 cm3/g at 5 kPa)capacities in the low-pressure region at 298 K were realized on Ni-MOF,suggesting the strong affinities of Ni-MOF towards C2H6 and C3H8.Furthermore,the dynamic breakthrough experiments revealed that purifying CH4 from natural gas in one-step can be achieved in Ni-MOF with high-purity(＞99.8％)and productivity(346.0 cm3/g).Most significantly,the production of Ni-MOF can be scalably synthesized at room temperature,rendering it promising potential for industrial application.The combined advantages of exceptional separation performance,scalability,and cycle stability of Ni-MOF pave the way for one-step CH4 purification from natural gas.
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    Supported Recyclable Metal-free Frustrated Lewis Pair Catalyst for Catalytic Hydrogenation of Substituted Pyridines to Piperidines

    MA ShaohuaTANG Zhiyong
    682-689页
    查看更多>>摘要：The construction of heterogeneous frustrated Lewis pairs(FLPs)catalysts is crucial for realizing highly efficient and recyclable pyridines catalytic hydrogenation.In this work,we prepared a recyclable heterogenous FLPs catalyst CMP-BF with conjugated microporous polymer CMP-ethynyl as the support via self-catalyzed 1,1-carboboration reaction with commercial Lewis acid B(C6F5)3.The as-synthesized CMP-BF demonstrates superior heterogenous catalytic hydrogenation performance(conversion＞99％),and considerable stability(84％conversion after three cycles)in recyclable hydrogenation of 2,6-phenylpyridine.This work provides insights into the fabrication and catalytic application of recyclable heterogenous FLP catalysts.
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    Balanced Polysulfide Containment and Lithium Ion Transport in Lithium-Sulfur Batteries via Nitrogen-doped Carbon Hollow Multi-shelled Structures on Modified Separators

    RAO FuXIAO QianWEI YanzeWANG Jiangyan...
    690-698页
    查看更多>>摘要：Representing the next-generation technology in lithium-ion batteries,lithium-sulfur(Li-S)batteries offer increased specific energy without relying on scarce metals like nickel and cobalt,but suffer from a low practical specific energy due to poor conductivity and a short lifespan due to the shuttle effect of polysulfides.Balancing the confinement of polysulfides and the transport of lithium ions requires highly elaborate modifiers for separators.Hollow multi-shelled structures(HoMS)show promise as hierarchical mesostructures for separators,offering multiple shell layers and internal cavities that effectively inhibit polysulfide shuttle.Thoughtful design of these structures is crucial to address these challenges effectively.In this study,nitrogen-doped carbon HoMS(NC HoMS)was created using polymer templates through a precisely controlled polymerization process.Batteries featuring NC HoMS-modified separators exhibit improved capacity and cycling stabi-ity in comparison to those utilizing commercial separators.Especially,triple-shelled NC HoMS strikes a balance in polysulfide containment and lithium ion transport.Featuring a sulfur loading of 6.34 mg/cm2,the Li-S battery can consistently complete 100 charge-discharge cycles,starting with a discharge capacity of 966.4 mA·h/g with a 75.8％capacity retention rate.NC HoMS holds potential as the separator modifier in addressing the polysulfide shuttle problem and facilitating the Li-ion transportation for advanced Li-S batteries.
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    Halogenated Thienoacene Derivatives with Improved Emission Properties

    ZHANG JingmeiMENG ZhihaoZHEN YonggangHE Ping...
    699-703页
    查看更多>>摘要：Thienoacenes is one of most important groups of semiconducting materials due to the high stability and superior mobility.However,there are scarce studies on the emission properties of thienoacenes to date.Herein,we synthesized fluorinated and chlorinated dibenzo[d,d']thieno[3,2-b;4,5-b']dithiophenes(DBTDTs)derivatives F6-DBTDT and C16-DBTDT by sulfoxide cyclization,significantly lowering the energy levels relative to the parent compound DBTDT.According to single crystal structure analysis,F6-DBTDT molecules adopt one-dimensional slipped stacking with close π-π interactions of 3.43 Å(1 Å=0.1 nm),which is different from the parent compound DBTDT with herringbone stacking motif.Interestingly,the halogenated DBTDT derivatives exhibit enhanced emission properties both in solution and in the solid state,opening up possiblities to improve photoluminescence of thienoacences by halogenation.
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    Hierarchically Macroporous Zeolite ZSM-5 Microspheres for Efficient Catalysis

    ZHENG MingdanCHEN YaLIU ZhanLYU Jiamin...
    704-711页
    查看更多>>摘要：Hollow zeolite microspheres have recently attracted much attention for their applications in catalysis,microreactors and biomedicine.Herein,we present hierarchically structured zeolite ZSM-5 microspheres with unique,abundant macropores that allow more efficient use for catalysis.The hierarchically macroporous zeolite ZSM-5 microspheres are synthesized under the assistance of water/oil emulsions and using polystyrene nanospheres as templates.The zeolite microsphere is assembled by uniform hollow zeolite nanospheres.Their large inner cavities and thin zeolite shells lead to smaller diffusion channel and higher improved accessibility to active sites,contributing to high catalytic performance in the catalytic conversion of benzyl alcohol in mesitylene.Such novel zeolite microspheres with impressive performance will be applied to numerous other industrial catalytic reactions.
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    Optimizing the π-Bridge of Non-fullerene Acceptors to Suppress Dark Current in NIR Organic Photodetectors

    SHAO LinHUANG YijunHONG LingXU Zishuo...
    712-721页
    查看更多>>摘要：Recently,the rapid development of non-fullerene acceptors(NFAs)has laid the foundation for performance improvements in near-infrared(NIR)organic photodetectors(OPDs).However,reducing the bandgap of NFAs to achieve strong absorption in the shorter-wave region usually leads to increased dark current density(Jd)and decreased responsivity(R),severely limiting the detectivity(D*)of NIR-OPDs.To date,it remains challenging to manipulate the Jd of NIR-OPDs through rational structure engineering of NFAs.Herein,three NIR-NFAs,namely bis(2-decyltetradecyl)4,4'-(2',7'-di-tert-butylspiro[cyclopenta[2,1-b:3,4-b']dithiophene-4,9'-fluorene]-2,6-diyl)bis(6-(((Z)-1-(dicyanomethylene)-5,6-difluoro-3-oxo-1,3-dihydro-2H-inden-2-ylidene)methyl)thieno[3,4-b]thiophene-2-carboxylate)(TSIC-4F),bis(2-decyltetradecyl)6,6'-(2',7'-di-tert-butylspiro[cyclopenta[2,1-b:3,4-b']dithiophene-4,9'-fluorene]-2,6-diyl)bis(4-(((Z)-1-(dicyanomethylene)-5,6-difluoro-3-oxo-1,3-d ihydro-2H-inden-2-ylidene)methyl)thieno[3,4-b]thiophene-2-carboxylate)(STIC-4F),and 2,2'-((2Z,2'Z)-(((2',7'-di-tert-butylspiro[cyclopenta[2,1-b:3,4-b']dithiophene-4,9'-fluorene]-2,6-diyl)bis(2,3-bis(5-(2-butyloctyl)thiophen-2-yl)thieno[3,4-b]pyrazine-7,5-diyl))bis(metha-neylylidene))bis(5,6-difluoro-3-oxo-2,3-dihydro-lH-indene-2,1-diylidene))dimalononitrile(TPIC-4F),were designed using the thieno[3,4-b]thiophene(TT)and thieno[3,4-b]pyrazine(TPy)derivatives as the it-bridge.Owing to the intramolecular S-S and S-N interactions,STIC-4F and TPIC-4F exhibited smaller backbone distortions than下SIC-4F.A significantly red-shifted absorption with a peak at 1015 nm was observed in TPIC-4F film,larger than that(ca.960 nm)for TSIC-4F and STIC-4F films.Moreover,OPDs operating in a photovoltaic mode were successfully fabricated,and TPIC-4F-based OPDs achieved the lowest Jd of 3.18×10-8 A/cm2 at-0.1 V.Impressively,although TPIC-4F-based OPDs exhibited the lowest R,higher shot-noise-limited specific detectivity(Dsh*)in 1000-1200 nm could be achieved due to its lowest Jd.This study underscored the effectiveness of optimizing the 7T-bridge structure of NFAs to suppress Jd,ultimately attaining higher Dsh* in the NIR region.
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    Multifunctional Sodium Gluconate Electrolyte Additive Enabling Highly Reversible Zn Anodes

    ZHAO KangZHAO JiananYU MengLIU Fangming...
    722-729页
    查看更多>>摘要：Sodium gluconate(SG)is reported as an electrolyte additive for rechargeable aqueous zinc batteries.The SG addition is proposed to modulate the nucleation overpotential and plating behaviors of Zn by forming a shielding buffer layer because of the adsorption priority and large steric hindrance effect,which contributes to limited rampant Zn2+diffusion and mitigated hydrogen evolution and corrosion.With the introduction of 30 mmol/L SG in 2 mol/L ZnS04 electrolyte,the Zn anode harvests a reversible cycling of 1200 h at 5 mA/cm2 and a high average Coulombic efficiency of Zn plating/stripping(99.6％).Full cells coupling Zn anode with V2O5·1.6H2O or polyaniline cathode far surpass the SG additive-free batteries in terms of cycle stability and rate capability.This work provides an inspiration for design of a high-effective and low-cost electrolyte additive towards Zn-based energy storage devices.
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    Reaction Kinetics and Secondary Organic Aerosol Composition Analysis of 2-Cyclohexen-1-one with NO3 Radicals

    HU LinTONG ShengruiXU YanyongZHANG Hailiang...
    730-736页
    查看更多>>摘要：Unsaturated ketones are typical oxygenated volatile organic compounds(OVOCs)with high reactivity,and are important precursors in air pollution.The sources of OVOCs are complex and include direct emissions and secondary oxidation formation of VOCs in the atmosphere.2-Cyclohexen-1-one is a widespread substance,and is derived from the industrial catalytic oxidation of cyclohexene.In this paper,we investigated the rate constants of the chemical reactions of 2-cyclohexen-1-one with NO3 radicals,which is(7.25±0.29)×10-15 cm3·molecule-1·s-1 at 298 K and under 1 atm(1 atm=101325Pa).It supplemented the kinetics of NO3 radicals database,and revealed its effects in the nighttime atmosphere.In addition,the reaction products of 2-cyclohexen-1-one with N03 radicals were detected by Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR MS),which revealed a series of nitrate esters in the composition of the secondary organic aerosol(SOA),which may reduce atmospheric visibility.Finally,the possible pathways for the generation of the products were developed.
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    MOF-derived 1D CGO Cathode for Efficient Solid Oxide Electrolysis Cells

    TIAN JiayuSUN QiLIU PeiDAI Jiuyi...
    737-746页
    查看更多>>摘要：Solid oxide electrolysis cells(SOECs)provide a promising way for converting renewable energy into chemical fuels.Traditionally,NiO/CGO(nickel-gadolinium doped ceria)cermet has shown its excellent properties in ionic and electronic conductivity under reducing conditions.Herein,we developed a novel 1D NiO/CGO cathode through a cerium metal-organic framework(MOF)derived process.The cathode's 1D nanostructure integrated with a microchannel scaffold facilitates enhanced mass transport,providing vertically aligned pathways for CO2 and H2O diffusion.Additionally,the 1D framework increases the number of interfacial sites and reduces ion diffusion distances,thereby simplifying electron/ion transport.Consequently,this advanced cathode achieved a significant breakthrough in SOEC performance,maintaining efficient CO2 and H2O electrolysis at an extraordinary current density of 1.41 A/cm2 at 1.5 V and excellent stability over 24 h at 850 ℃.The enhanced performance of this newly developed cathode not only achieves a remarkable 100％improvement compared to those of NiO/CGO cathodes with varying geometrical configurations but also surpasses those of commercial NiO/CGO catalysts by an outstanding 40％when tested under identical conditions.The development of the 1D NiO/CGO enhances the efficiency and durability of ceramic cathodes for CO2 and H2O co-electrolysis in SOECs and improves the scalability and effectiveness of SOECs in renewable energy applications.
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