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Green Chemical Engineering 2024年第4期5卷 409-417页

作者： Yu Chen Zhiwu Yu MOE Key Laboratory of Bioorganic Phosphorous chemistry and Chemical Biology Department of ChemistryTsinghua University

Green solvents such as water and ionic liquids(iLs) are pillars of the great mansion of green chemistry and green processing. initially proposed as a new family of iLs,deep eutectic solvents(DESs) have received fast development in the past two decades. in this contribution,DESs are reviewed critically and the concept is extended to lowmelting mixture solvents(Lo MMSs),which cover all kinds of materials including ionic compounds,molecular compounds,and metals. Six classes of Lo MMSs are proposed as the new classification system and examples are given. Finally,several thermodynamic issues concerning Lo MMSs are discussed. Two new concepts,robustness of Lo MMSs and high-entropy Lo MMSs,are proposed.

关键词： Green solvents Deep eutectic solvents Low transition temperature mixture solvents Phase diagram EGain

increase of chiral sensing ability in host-guest chemistry by magnetic anisotropy

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Science China chemistry 2024年第8期67卷 2775-2782页

作者： Jia-Liang Chen Bin Li Feng Yang Tiesheng Shi Xun-Cheng Su State Key Laboratory of Elemento-organic chemistry Tianjin Key Laboratory of Biosensing and Molecular RecognitionCollege of ChemistryNankai UniversityTianjin 300071China College of chemistry Chemical Engineering and Materials ScienceZaozhuang UniversityZaozhuang 277160China

Enantiomeric molecules generally play distinct functions in chemistry,biology,and *** physical and chemical properties of chiral analytes lay difficulty in discrimination and quantification of the *** report herein an efficient approach of increasing the chiral sensing ability ofβ-cyclodextrin(β-CD),a widely used host molecule,in the hostguest chemistry by magnetic anisotropy.A rigid and chiral lanthanide binding tag was attached to theβ-CD to amplify the changes of nuclear magnetic resonance(NMR)signals in the host-guest recognition *** installation of the paramagnetic lanthanide ion inβ-CD greatly enhances the enantiomeric discrimination up to 30-fold in comparison with the diamagneticβ-CD *** addition,the magnitude of the paramagnetic effects is tunable according to the diverse range of paramagnetic strength of the lanthanide *** reported method significantly increases the chiral sensing ability ofβ-CD,which can be applied to other host *** transferred paramagnetic effects,pseudocontact shifts(PCSs)and paramagnetic relaxation enhancements(PREs),from the host to the guest molecules,are valuable structural restraints to determine the absolute stereochemistry of the chiral *** strategy does not need modification of the analytes and is complementary to the reported analytical methods that rely on the functionalization of the chiral analytes.

关键词： chiral recognition nuclear magnetic resonance host-guest chemistry magnetic anisotropy lanthanide ions

Layered oxide cathodes for sodium-ion batteries:microstructure design,local chemistry and structural unit

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Science China chemistry 2024年第1期67卷 191-213页

作者： Ling-Yi Kong Han-Xiao Liu Yan-Fang Zhu Jia-Yang Li Yu Su Hong-Wei Li Hai-Yan Hu Yi-Feng Liu Ming-Jing Yang Zhuang-Chun Jian Xin-Bei Jia Shu-Lei Chou Yao Xiao institute for Carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China

Because of the low price and abundant reserves of sodium compared with lithium,the research of sodium-ion batteries(SiBs)in the field of large-scale energy storage has returned to the research *** oxides distinguish themselves from the mains cathode materials of SiBs owing to their advantages such as high specific capacity,simple synthesis route,and environmental ***,the commercial development of the layered oxides is limited by sluggish kinetics,complex phase transition and poor air *** on the research ideas from macro-to micro-scale,this review systematically summarizes the current optimization strategies of sodium-ion layered oxide cathodes(SLOC)from different dimensions:microstructure design,local chemistry regulation and structural unit *** the dimension of microstructure design,the various structures such as the microspheres,nanoplates,nanowires and exposed active facets are prepared to improve the slow kinetics and electrochemical ***,from the view of local chemistry regulation by chemical element substitution,the intrinsic electron/ion properties of SLOC have been enhanced to strengthen the structural ***,the optimization idea of endeavors to regulate the physical and chemical properties of cathode materials essentially is put forward from the dimension of structural unit *** opinions and strategies proposed in this review will provide some inspirations for the design of new SLOC in the future.

关键词： sodium-ion batteries layered oxide cathodes microstructure design local chemistry structural unit

Who is Who in the Carbene chemistry of N-Sulfonyl Hydrazones

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Chinese Journal of chemistry 2024年第17期42卷 2071-2108页

作者： Paramasivam Sivaguru Yongzhen Pan Nan Wang Xihe Bi Departmentof chemistry Northeast Normal UniversityChangchunJilin130024China

Over the past few decades,N-sulfonyl hydrazones have been recognized as alternative precursors for hazardous diazo compounds in organic synthesis,allowing for diverse innovative and original chemical transformations that were otherwise difficult to *** critical review summarizes the major advancements in the carbene chemistry of N-sulfonyl *** contents of this review are organized based on research conducted by leading scientists who have made significant contributions to this *** individual carbene transfer reactions and their mechanisms,as well as the potential applications in the synthesis of natural products and complex bioactive molecules,are thoroughly discussed.

关键词： N-Sulfonyl hydrazones Carbene chemistry Cross-coupling Cycloaddition Asymmetric reactions

Self-separation ionic liquid catalyst for the highly effective conversion of H2S by α,β-unsaturated carboxylate esters under mild conditions

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Green Energy & Environment 2024年第9期9卷 1440-1448页

作者： Wenjie Xiong Xiaomin Zhang Xingbang Hu Youting Wu Key Laboratory of Mesoscopic chemistry of MOE School of Chemistry and Chemical Engineering Nanjing University The institute of Green chemistry and Engineering School of Chemistry and Chemical Engineering Nanjing University

The deep-processing utility of pure hydrogen sulfide （H2S） is a significant direction in natural gas chemical ***,a brand-new strategy of H2S conversion by a,β-unsaturated carboxylate esters into thiols or thioethers using task-specific carboxylate ionic liquids （iLs） as catalyst has been developed,firstly accomplishing the phase separation of product and catalyst without introducing the third *** can be considered as a cascade reaction in which the product selectivity can be controlled by adjusting the molar ratio of H2S to a,β-unsaturated carboxylate ***,the effects of iLs with different anions and cations,intermittent feeding operations,as well as pressure-time kinetic behaviors on cascade reaction were ***,the proposed interaction mechanism of H2S conversion using butyl acrylate catalyzed by[Emim][Ac]was revealed by DFT-based theoretical *** approach enables the self-phase separation promotion of catalyst and product and achieves 99%quantitative conversion under mild conditions in the absence of solvent,making the entire process ecologically ***-efficiency reaction activity can still be maintained after ten cycles of the ***,the good results,combined with its simplicity of operation and the high recyclability of the catalyst,make this green method environmentally friendly and *** is anticipated that this self-separation method mediated by task-specific iLs will provide a feasible strategy for H2S utilization,which will guide its application on an industrial scale.

关键词： ionic liquid Cascade reaction Self-separation H 2 S conversion Catalysis

The 4^(th)CCL Organic chemistry Forum held in Zhangye

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Chinese Chemical Letters 2024年第8期35卷 3-6页

作者： Yingxiao Zong Yangfei Wei Xiaoqing Liu Junke Wang Huanfang Guo Junli Wang Zhuangzhi Shi Tao Tu Cheng Yang Chongyang Wang Leyong Wang Key Laboratory of Hexi Corridor Resources Utilization of Gansu School of Chemistry and Chemical EngineeringHexi UniversityZhangye 734000China institute of Materia Medica Chinese Academy of Medical SciencesBeijing 100050China School of chemistry and Chemical Engineering Nanjing UniversityNanjing 210023China Department of chemistry Fudan UniversityShanghai 200438China College of chemistry Sichuan UniversityChengdu 610064China institute of chemistry Chinese Academy of SciencesBeijing 100190China

The first Chinese Chemical Letters(CCL)Organic chemistry Forum was held in Xiamen of Fujian in Jan.2018,followed by the successful events in Zhengzhou of Henan in Dec.2019 and Linzhi of Tibet in July *** series of forums aim to build a high-level organic chemistry academic exchange platform for(Chinese)youthful organic chemists,fully showcase their latest fron-tier achievements,and enhance the international level of organic chemistry in *** the same time,the convening of the series of forums has also played a positive role in promoting the devel-opment of China’s scientific journal publishing,accelerating the re-alization of the strategic goal of building a world-class journal.

关键词： journal Forum Xiamen

Surface reconstruction and structural transformation of twodimensional Ni-Fe MOFs for oxygen evolution in seawater media

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Nano Research 2024年第4期17卷 2429-2437页

作者： Liyuan Xiao Xue Bai Jingyi Han Tianmi Tang Siyu Chen Hui Qi Changmin Hou Fuquan Bai Zhenlu Wang Jingqi Guan institute of Physical chemistry College of ChemistryJilin UniversityChangchun 130021China The Second Hospital of Jilin University Changchun 130021China State Key Laboratory of inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China Laboratory of Theoretical and Computational chemistry Institute of Theoretical ChemistryCollege of ChemistryChangchun 130023China

As a four-electron transfer reaction,oxygen evolution reaction(OER)is limited by large overpotential and slow ***,we in-situ synthesized two-dimensional(2D)Ni-Fe metal-organic framework nanosheets on nickel foam(NixFe-TPA/NF,TPA=terephthalic acid)for oxygen evolution in alkaline and alkaline seawater *** 1 M KOH,Ni3Fe-TPA/NF shows a low overpotential(η10)of 189 mV at 10 mA·cm^(-2) and an ultra-low overpotential of only 260 mV at 500 mA·cm^(-2).in alkaline seawater,Ni3Fe-TPA/NF still provides impressive OER performance,with anη10 of 265 ***-situ Raman characterization results show that the phase transition occurs during the OER,and Ni3FeOOH with more oxygen vacancies is in-situ formed,reducing the OER energy *** functional theory(DFT)reveals that the synergy between Ni and Fe reduces the energy barrier and accelerates the rate-determining *** addition,the ultra-thin 2D sheet structure and the close combination of Ni3FeOOH and highly conductive NF support ensure the high catalytic OER ***,the surface reconstruction and structural modification strategy can be used to design and prepare high-performance OER electrocatalysts for energy-related applications.

关键词： density functional theory(DFT)calculation Ni3FeOOH oxygen evolution reaction seawater electrolysis surface reconstruction

A Golden Touch in the Design of Multifunctional Porphyrin Metallacages:Host-Guest chemistry for Drug-Target interactions

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CCS chemistry 2024年第7期6卷 1662-1671页

作者： Tamara Rodríguez-Prieto Darren Wragg Nicole Heiduk Mihyun Park Nicole Strittmatter Roland A.Fischer Angela Casini Guillermo Moreno-Alcántar Chair of Medicinal and Bioinorganic chemistry Department of ChemistrySchool of Natural SciencesTechnical University of Munich85748 Garching b.München Professorship for Analytical chemistry Department of ChemistrySchool of Natural SciencesTechnical University of Munich85748 Garching b.München Chair of inorganic and MetalOrganic chemistry Department of ChemistrySchool of Natural SciencesTechnical University of Munich85748 Garching b.München Munich Data Science institute(MDSi) Technical University of Munich85748 Garching b.München

The use of three-dimensional self-assembled metallacages(MCgs)as multimodal drug platforms holds great ***,the synthesis of MCgs with increased complexity and functionality is a great challenge since understanding of the interaction of MCgs with biological targets is still *** this context,this work reports on the integration of a gold(iii)porphyrin scaffold into a prismatic MCg structure and explores its application for multimodal therapy of cancer in vitro,namely enabling both photodynamic therapy and *** experimental approaches with a state-of-the-art metadynamics theoretical study,we discovered that the gold cage shows unprecedented host-guest interaction-driven selective stabilization of guanine-quadruplex(G4)structures-validated anticancer drug targets-disclosing a new mechanism to pursue in the design of supramolecular drugs.

关键词： gold metallacages porphyrins G4stabili-zation host-guestchemistry anticanceragents

Combination of methylthio-chemistry with living crystallization-driven self-assembly toward uniformπ-conjugated nanostructures with antibacterial activity,surface tailorability,tunable morphology and dimension

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Science China chemistry 2024年第7期67卷 2341-2352页

作者： Chuyu Duan Binbin Xu Ruru Li Xiaoyu Huang Shaoliang Lin Chun Feng Shanghai Key Laboratory of Advanced Polymeric Materials School of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China School of chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China Key Laboratory of Fluorine and Nitrogen chemistry and Advanced Materials Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Living crystallization-driven self-assembly(CDSA)provides robust access to uniformπ-conjugated nanostructures(CNSs)from block copolymers(BCPs)containing a crystallineπ-conjugated segment with controlled dimension,morphology and composition,which show appealing applications in biomedicine,photocatalysis and *** further expand the application spectrum of these CNSs,the development of facile strategies toward diverse CNSs with varying structures/functionalities is highly ***,BCPs consisting of oligo(p-phenylene ethynylene)-b-poly(polypropyl-3-methanethiol acrylate)(OPE_(9)-bPMTPA35and OPE_(9)-b-PMTPA_(58);the subscript represents the number of repeat unit of each block)consisting of a crystallineπ-conjugated core-forming OPE_(9)segment and a corona-forming PMTPA block are *** efficient“click-type”alkylation of methylthio groups,OPE_(9)-b-PMTPA with varying contents of sulfonium unit is *** ribbon-like micelles with different widths and lengths can then be generated in a controlled manner via the self-seeding approach of living ***,negatively charged polymeric and Ag nanoparticles can be immobilized on sulfonium/methylthio-containing shells by taking advantage of electrostatic attraction and coordination interaction,***,the ribbon-like micelles with positively charged shells exhibit antibacterial activity against *** the ease of modification of PMTPA-based shell and attractive opto-electronic/photocatalytic properties ofπ-conjugated units,the combination of methylthio-chemistry and living CDSA opens a new avenue to generate multi-functional CNSs for widespread applications from biomedicine to photocatalysis.

关键词： crystallization-driven self-assembly block copolymer π-conjugated nanostructure methylthio-chemistry

Multicolor circularly polarized phosphorescence of axially chiral binuclear platinum(Ⅱ) complexes

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Science China chemistry 2024年第11期67卷 3757-3766页

作者： Jintong Song Rui Zeng Hui Xiao Hailiang Ni Zong-Xiang Xu Haifeng Xiang College of chemistry and Materials Science Sichuan Normal University Department of chemistry Southern University of Science and Technology College of chemistry Sichuan University

D-A charge transfer, including through-bond charge transfer and through-space charge transfer between two different electron donors（D） and electron acceptors（A）, is a fundamental and powerful tool to tune the optical properties of organic dyes. Herein,we demonstrate a unique strategy to tune phosphorescence and circularly polarized luminescence properties of axially chiral binuclear Pt（Ⅱ） complexes through long-range charge transfer, even though these molecules have two totally identical segments on either side of the chiral core. The presence of axial chirality would break not only the symmetry of molecular structure and π-conjugation system but also the symmetry of charge distribution for long-range charge transfer. These binaphthyl-based Pt（Ⅱ）complexes bearing coordinated atoms far away from chiral axis exhibit no Pt-Pt interactions but colorful concentrationdependent phosphorescence with quantum yield up to 86.4% and could be applied as emitters in highly efficient solutionprocessed organic light-emitting diodes to achieve luminance, luminance efficiency, power efficiency, external quantum efficiency, and asymmetry factor up to 8.94 × 10～3cd m-2, 41.9 cd A-1, 18.8 lm W-1, 12.6% and 2.98 × 10-3, respectively. Therefore,the present work affords a new and simple way to utilize the inherently asymmetric advantage of chirality for the design of D-Abased organic dyes.

关键词： Pt(ii) complexes organic light-emitting diodes circularly polarized phosphorescence axial chirality