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1,3-Dipolar Cycloaddition of Polycyclic Aromatic Azomethine Ylides and Alkynylbenziodoxoles for Synthesis of Functional Dibenzoullazines

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Chinese Journal of chemistry 2024年第10期42卷 1079-1083页

作者： Hui Han Glen Wee Zhuan Goh Yongxin Li Naohiko Yoshikai Shingo Ito schoolof chemistry ChemicalEngineering and BiotechnologyNanyang Technoogical University21 Nanyang LinkSingapore 637371Singapore Graduate School of Pharmaceutical Sciences Tohoku UniversitySendai 980-8578Japan

A new family of dibenzoullazine derivatives was synthesized through 1,3-dipolar cycloaddition of polycyclic aromatic azomethine ylides with alkynylbenziodoxoles followed by oxidation.The benziodoxole moiety in the resulting products was used as a versatile linchpin for the synthesis of structurally diverse functional dibenzoullazines that are difficult to access by other synthetic methods.

关键词： Cycloaddition Nitrogen heterocycles Azomethine ylides Hypervalent compounds Dibenzoullazine

Effect of Hyperconjugation on Photovoltaic Performance in Pseduo-2D Perylene Diimide Derivatives

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Chinese Journal of chemistry 2024年第7期42卷 725-730页

作者： Zhilong He Yuwen Hong Guangyu Li Tong Shan Yi Zhang Hongliang Zhong schoolof chemistry and Chemical Engineering Shanghai Key Lab of Electrical Insulation and Thermal AgingShanghai Jiao Tong UniversityShanghai200230China Shanghai Institute of Organic chemistry Chinese Academy of SciencesShanghai 200032China Shenzhen Research institute Shanghai Jiao Tong UniversityShenzhenGuangdong 518057China

Theπ-πinteraction is acknowledged as the predominant factor to determine the molecular packing in organic photovoltaic materials,while other non-covalent intermolecular interactions especially theσ-πhyperconjugation are often ignored.Herein,a perylene diimide(PDI)derivative named FIDT-PDI is designed and synthesized to shed light into the effect of hyperconjugation on the molecular packing and further the photovoltaic performance.Dynamic NMR and 2D NOE NMR demonstrate the formation of intermolecularσ-πhyperconjugation between the C—H bond of the PDI moiety in one molecule and the phenyl sidechain in another molecule of FIDT-PDI.Benefiting from theσ-πhyperconjugation,FIDT-PDI with twisted backbone reversely exhibits more ordered packing and stronger crystallinity compared with another PDI derivative FIDTT-PDI which has better planarity,consequently achieving superior PCE and higher carrier mobility.This contribution is the first paradigm to unravel the structure-property relationship betweenσ-πhyper-conjugation of conjugated materials and corresponding photovoltaic performance.

关键词： Hyperconjugation Weak intermolecular interactions Conformation Organic solar cells Nonfullerene acceptor Perylene diimide

Direct Analysis of Whole Blood by a Disposable Monolithic Column Mass Spectrometry Analysis Kit

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Chinese Journal of chemistry 2024年第10期42卷 1073-1078页

作者： Wenxin Wang Jin Han Yutong Zheng Haijie Wang Chengbiao Zhu Yongyi Li Yuqi Feng Zhenwei Wei Xiangyu Wang College of chemistry and Molecular Science Wuhan UniversityWuhanHubei 430072China School of Public Health Wuhan UniversityWuhanHubei 430072China schoolof Bioengineering and Health Wuhan Textile UniversityWuhanHubei 430200China

A monolithic column-based mass spectrometry(MS)analysis kit was prepared for whole blood analysis with MS.The kit is disposable and can be used for purification,storage,transportation and direct analysis of whole blood.The kit mainly consists of a capillary for quantitative microsampling,a cation exchange monolithic column for purification and storage,and a syringe for loading sample.This kit is very friendly to various users that one can easily siphon the blood in the kit followed by rapid clean-up.We established a quantitative method using the kit with a limit detection as low as 0.33 nmol/L,and achieved more than five orders of magnitude enhancement in sensitivity compared to direct nanoelectrospray ionization MS analysis.The column can avoid analyte exposure to environment,which helps the storage of the sample for laboratory analysis.The relative standard deviation of immediate blood analysis and storage blood analysis within 10 d was less than 10%.This method has been successfully applied to the quantitative analysis of procainamide hydrochloride in 2μL rat blood.These results indicate that this disposable kit does have the potential to achieve highly sensitive quantitative MS analysis in biological samples,which is expected to become a cost-effective and powerful tool for in vitro diagnostics.

关键词： Clinical Ms Whole blood analysis Porous polymers Matrix isolation Trace analysis

Immobilizing Triphenylamine with Photoredox Inert Sr^(2+)Forming Sr-MOF with Controlled Electron Migration for Photocatalytic Oxidation of Thiols to Disulfides

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Chinese Journal of chemistry 2024年第10期42卷 1093-1099页

作者： Ying-Xia Wang Fang Zheng Dong-Xia Song Bao-Yue Niu Lu-Qian Deng Xian-Ming Zhang Key Laboratory of Magnetic Molecules and Magnetic Information Materials(Ministry of Education) Schoolof Chemistry and Materials ScienceShanxi Normal UniversityTaiyuanShanxi 030006China Key Laboratory of Interface Science and Engineering in Advanced Material(Ministry of Education) College of ChemistryTaiyuan University of TechnologyTaiyuanShanxi 030024China

The photocatalytic oxidative coupling of thiols is one of the most popular methods to synthesize the disulfides.Triphenylamine and its derivatives(TPAs)are promising for the above reaction,but suffer from the easy polymerization and difficult separation.To overcome these obstacles while controlling the photogenerated electrons transfer directly to target substrates,herein,we constructed one TPA-based metal-organic framework(MOF),(Me_(2)NH_(2))[Sr(TCBPA)]·DMA·3H_(2)O(1),by direct self-assembly of tris(4′-carboxybiphenyl)amine(H_(3)TCBPA)and photoredox inert strontium ion(Sr^(2+)).DFT calculations revealed that the valence band maximum(VBM)and the conduction band minimum(CBM)are mainly located on TCBPA^(3-),successfully inhibiting the undesirable electron migration to metal nodes.Experimental results indicated that 1 displays superior performance than homogeneous H_(3)TCBPA,which may result from the abundant π…π and C—H…π interactions between the well-arranged TCBPA^(3-)and the build-in electric field between the anionic framework and the Me_(2)NH^(2+).This work highlights that immobilizing TPAs into MOFs is one promising approach to designing heterogeneous photocatalysts for the synthesis of disulfides by oxidative coupling of thiols.

关键词： Triphenylamine Metal-organic frameworks Strontium Photooxidation Thiols Disulfides

MoS2-based anode materials for lithium-ion batteries:Developments and perspectives

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Particuology 2024年第4期87卷 240-270页

作者： Lianyu Zhao Yishan Wang Chuncheng Wei Xiaoxiao Huang Xueqian Zhang Guangwu Wena School of Materials Science and Engineering Shandong University of TechnologyZibo255000China schoolof Materials Science and Engineering Harbin Institute of TechnologyHarbin10001China

In recent years,significant progress has been achieved in the creation of innovative functional materials for energy storage and conversion.Due to their distinct physicochemical characteristics,ultrathin nanosheets composed of common layered transition metal sulfide materials(MoS2)have demonstrated promise as high-capacity anode materials for lithium-ion batteries(LIBs).Nevertheless,their practical application is severely limited by the tendency of monolayer nanosheets to restack due to strong van der Waals forces,dramatic volume changes during successive cycles,and low intrinsic conductivity.Recent research advances have shown that composite structures and nanowire morphologies with specific morphologies effectively overcome these issues.This paper reviews the recent research progress on molybdenum disulfide-based composites as anode materials for LIBs and discusses in detail the struc-tural characteristics of pure molybdenum disulfide and other composite forms of molybdenum disulfide.In addition,the phase engineering,defect engineering,and lithium storage mechanisms of molybdenum disulfide and the synthesis of molybdenum disulfide-based nanocomposites by different preparation methods are focused on.Finally,we review the design(structure),recent developments,and challenges of novel anode materials and consider their electrochemical performance in Li-ion batteries.

关键词： Lithium-ion battery MoS_(2)-Based anode composites Synthesis methods Defect engineering Lithium storage mechanism

Thermoelectric Properties of an Indandione-Terminated Quinoidal Compound:Effect of the n-Type Dopants

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Chinese Journal of chemistry 2024年第9期42卷 997-1003页

作者： Yingying Liu Cheng Wang Tianzuo Wang Fei Jiao Shaoqiang Dong Yunfeng Deng Yanhou Geng School of Materials Science and Engineering and Tianjin Key Laboratory of Molecular Optoelectronic Science Tianjin Universityand Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin 300072China Institute of Molecular Aggregation Science Tianjin UniversityTianjin 300072China Tianjin Key Laboratory of Molecular Optoelectronic Science Department of ChemistrySchoolof ScienceTianjin UniversityTianjin300072China Joint schoolof NationalUniversity of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New City FuzhouFujian350207China

The investigation of n-type doping holds a significant interest for the application of thermoelectrics.Herein,the doping of an indandione-terminated compound Q-4F with a singlet open-shell ground state was studied using two n-dopants N-DMBI and LCV.Both of these two dopants can effectively dope Q-4F due to the large offset between the singly occupied molecular orbital(SOMO)of dopants and the lowest unoccupied molecular orbital(LUMO)of Q-4F.N-DMBI has a higher doping ability than LCV as demonstrated by the UV-vis-NIR and EPR measurements.However,in comparison to N-DMBI doped Q-4F,LCV doped system exhibits much higher electrical conductivity and power factor due to its unperturbed molecular packing and favorable morphology after doping.The optimal conductivity of LCV doped Q-4F is 7.16×10^(-2)±0.16 S·cm^(-1) and the highest power factor reaches 12.3±0.85μW·m–1·K^(-2).These results demonstrate that the modulation of n-dopants is a powerful strategy to balance the doping efficiency and microstructure toward a maximum thermoelectric performance.

关键词： n-Doping Indandione Quinoidal compounds Organic thermoelectrics Electron transfer Organic electronics Energy conversion

Influence of crystal-transforming agent on the performance and mechanism ofα-high-strength gypsum prepared from FGD gypsum

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Particuology 2024年第4期87卷 37-45页

作者： Zhuoyue Xu Xiao Wang Biao Jin Dawang Zhang Hui Li College of Materials Science and Engineering Xi'an University of Architecture and TechnologyXi'an710055China schoolof Materials and Chemical Engineering Henan University of Urban ConstructionPingdingshan46736China

This paper investigates the impact of flue gas desulfurization(FGD)gypsum's crystal modifier on the characteristics and microcosmic mechanism ofα-high strength gypsum.The results demonstrate that all three crystal modifiers can convert FGD gypsum toα-high-strength gypsum.Citric acid(CA)has the most significant influence onα-high-strength gypsum,and the preparedα-high-strength gypsum is short columnar,with an aspect ratio in the range of 1-3,and has a faster setting time,a larger specific surface area,and a smaller standard consistency,higher compressive strength,greater surface hardness,and smaller crystal particle size.The initial setting time of theα-high-strength gypsum manufactured with CA crystal modifier was decreased by 36%compared to the blank sample,the final setting time was lowered by 37.5%,and the water consumption of the standard consistency was reduced by 8%.The maximum strength is 32 MPa after 2 h,the absolute dry compressive strength is up to 38 MPa,and the surface hardness is improved by 24.43%.

关键词： Flue gas desulfurization gypsum Crystal modifier Microscopic mechanism α-high-strength gypsum

Design of Support Effect in the Catalytic Application of Ligand-Protect Gold Clusters

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Chinese Journal of chemistry 2024年第1期42卷 73-86页

作者： Shuohao Li Shenguang Fu Yuqing Gong Nuojie Wu Lei Wang Liang Wang School of Safety Engineering China University of Mining and TechnologyXuzhouJiangsu 221116China schoolof chemistry and Chemical Engineering Yangzhou UniversityYangzhouJiangsu 225009 Jiangsu Key Laboratory of Coal-based Greenhouse Gas Control and Utilization China University of Mining and Technology XuzhouJiangsu 221008China

Ligand-protected gold(Au_(n))clusters sometimes need the removal of organic ligands to expose more active sites and reduce steric hindrance in catalytic reactions,and large amount of organic and inorganic materials usually need to be employed as supports to anchor Aun clusters through different interaction mechanisms.Whereas,less comprehensive summaries have been provided about the crucial contribution of various supports to the catalytic performance of the supported Aun clusters.Herein,this review firstly summarizes synthesis methods(e.g.,impregnation and encapsulation processes)for the supported Aun cluster catalysts,and then mainly points out specific contributions of support effect in a great diversity of catalytic reactions,as well as deep interaction mechanisms.Besides,opportunities and challenging issues will be stated towards supported Aun clusters,in terms of improving catalytic performance and structural stability of Aun clusters inthedemand of catalysis.

关键词： Gold clusters Synthesis Support effect Catalytic performance Interaction

Photocatalytic seawater splitting by 2D heterostructure of ZnIn_(2)S_(4)/WO_(3) decorated with plasmonic Au for hydrogen evolution under visible light

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Journal of Energy chemistry 2024年第6期93卷 55-63,I0003页

作者： Huiqin An Yanjun Wang Xing Xiao Jiaxin Liu Zhiyao Ma Tianxin Gao Wanyu Hong Lizhi Zhao Hong Wang Qingjun Zhu Shanshan Chen Zhen Yin School of chemistry Tiangong UniversityTianjin 300387China School of Materials Science and Engineering Tiangong UniversityTianjin 300387China Deutsches Elektronen-Synchrotron DESY 15738 ZeuthenGermany schoolof Materials Science and Engineering & National Institutefor Advanced Materials Nankai University Tianjin300350 China College of Chemical Engineering and Materials Science Tianjin University of Science and TechnologyTianjin 300457China

Photocatalytic H_(2) evolution from seawater splitting presents a promising approach to tackle the fossil energy crisis and mitigate carbon emission due to the abundant source of seawater and sunlight on the earth.However,the development of efficient photocatalysts for seawater splitting remains a formidable challenge.Herein,a 2D/2D ZnIn_(2)S_(4)/WO_(3)(ZIS/WO_(3))heterojunction nanostructure is fabricated to efficiently separate the photoinduced carriers by steering electron transfer from the conduction band minimum of WO_(3) to the valence band maximum of ZIS via constructing internal electric field.Subsequently,plasmonic Au nanoparticles(NPs)as a novel photosensitizer and a reduction cocatalyst are anchored on ZIS/WO_(3) surface to further enhance the optical absorption of ZIS/WO_(3) heterojunction and accelerate the catalytic conversion.The obtained Au/ZIS/WO_(3) photocatalyst exhibits an outstanding H_(2) evolution rate of 2610.6 or 3566.3μmol g^(-1)h~(-1)from seawater splitting under visible or full-spectrum light irradiation,respectively.These rates represent an impressive increase of approximately 7.3-and 6,6-fold compared to those of ZIS under the illumination of the same light source.The unique 2D/2D structure,internal electric field,and plasmonic metal modification together boost the photocatalytic H_(2) evolution rate of Au/ZIS/WO_(3),making it even comparable to H_(2) evolution from pure water splitting.The present work sheds light on the development of efficient photocatalysts for seawater splitting.

关键词： Photocatalytic seawater splitting 2D/2D ZnIn_(2)S_(4)/WO_(3) Surface plasmon resonance effect Interfacial electric field