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Unusual Single Electron Transfer Reactions between Alkenes and Iodine Electrophiles

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Chinese Journal of chemistry 2024年第5期42卷 471-477页

作者： Zhengzhao Lou Jingyu Hu Chuanfa Ni Xiu Wang Jinbo Hu Key lab.ratory of organofluorine chemistry Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of Sciences345 Ling Ling RoadShanghai200032 China School of Physical Science and Technology ShanghaiTech University100 Haike RoadShanghai201210 China

The electrophilic addition to an alkene with an electrophile has been widely studied and applied in organic *** organic chemistry textbook describes the classical reaction between an alkene and an iodine electrophile(such as elemental iodine and N-iodosuccinimide(NIS))as a typical ionic reaction,in which an iodonium ion is formed and then attacked by a ***,in this article,we report a new and unusual reaction mode between an alkene and NIS;that is,a single electron transfer(SET)process occurs between these two reactants by forming an electron-donor acceptor *** only does this unusual single electron transfer reaction between an alkene and NIS add fundamentally important knowledge to organic chemistry,it also provides a valuable synthetic method as the new SET reaction mode with opposite regioselectivity as compared with the traditional ionic mode.

关键词： Electrophilic addition Radical ions Reaction mechanisms Alkenes Fluorine

Rapid and chemoselective imidation of sulfides in aqueous buffer enabled by a novel guanidine-derived N-O reagent

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Science China chemistry 2024年第6期67卷 1929-1934页

作者： Hanzheng Li Long Xu Jiajia Dong Key lab.ratory of organofluorine chemistry Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai200032China Institute of Translational Medicine National Facility for Translational Medicine(Shanghai)Shanghai Jiao Tong UniversityShanghai200240China School of chemistry and Chemical Engineering Zhangjiang Institute for Advanced StudyShanghai Jiao Tong UniversityShanghai200240China Shanghai Artificial Intelligence lab.ratory Shanghai200232China

Herein we report the facile synthesis of a series of novel N-O reagents and identify N′-di-Boc-N′′-[(mesitylsulfonyl)oxy]-guanidine as an efficient imidating *** reagent is synthetically scalab.e and bench-stable,yet it shows unprecedented reactivity and chemoselectivity towards S(II)in buffer/hexafluoroisopropanol(HFIP)system,to generate a new class of Nguanyl *** transformation of N-guanyl sulfilimines to N-guanyl sulfoximines provides us a chance to investigate these rarely reached compounds,which are shown to be versatile precursors to a variety of N-heterocyclic and *** work provides an addition to the tool box of both sulfur imidation and guanidine synthesis,especially for the need of rapid and selective modifications of sulfur(II)center under biocompatible conditions.

关键词： sulfur imidation N-O reagent

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Efficient capture of difluorocarbene by pyridinium 1,4-zwitterionic thiolates:A concise synthesis of difluoromethylene-containing 1,4-thiazine derivatives

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Chinese Chemical Letters 2024年第4期35卷 367-370页

作者： Zhiwei Chen Heyun Sheng Xue Li Menghan Chen Xin Li Qiuling Song Institute of Next Generation Matter Transformation College of Materials Science&Engineering and College of Chemical Engineering at Huaqiao UniversityXiamen 361021China Fujian University Key lab.ratory of Molecule Synthesis and Function Discovery College of ChemistryFuzhou UniversityFuzhou 350108China State Key lab.ratory of Organometallic chemistry and Key lab.ratory of organofluorine chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

A practical method for the construction of difluoromethylene-containing 1,4-thiazine moieties using readily availab.e diethyl bromodifluoromethanephosphonate(BrCF_(2)PO(OEt)_(2))as difluorocarbene precusor has been *** transformation features the efficient capture of difluorocarbene by pyridinium 1,4-zwitterionic thiolates.A series of structurally novel and functionalized difluoromethylene-containing 1,4-thiazine derivatives were thus synthesized in good yields.

关键词： Difluoromethylene Pyridinium 1 4-zwitterionic thiolates 1 4-Thiazine derivatives

Pentacoordinate Phosphoranes as Versatile Reagents in Fluoroalkylation Reactions

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CCS chemistry 2024年第1期6卷 165-176页

作者： Huanhuan Song Weihao Li Xiaoying Wang Kaiteng Wang Jingwen Li Shuai Liu Pin Gao Xin-Hua Duan Jinbo Hu Mingyou Hu School of chemistry Engineering Research Center of Energy Storage Materials and DevicesMinistry of EducationXi’an Key Laboratory of Sustainable Energy Material ChemistryXi’an Jiaotong UniversityXi’an 710049 Key lab.ratory of organofluorine chemistry Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai 200032

A general method for the synthesis of bench-stable bis(difluoromethyl)pentacoordinate phosphoranes has been *** reaction is rapid,operationally simple,and easily *** pentacoordinate phosphoranes can generate both difluoromethyl radical(·CF_(2)H)and difluorocarbene(:CF_(2))***,a variety of fluoroalkylation transformations havebeen achieved by·CF_(2)H,such asoxidativedifluoromethylation of electron-deficient heterocycles,nickel/photoredox dual-catalyzed difluoromethylation of aryl bromides,and photoredox difluoromethylation of alkenes,or by:CF_(2),such as gem-difluorocyclopropanation of alkenes,base-promoted difluoromethylation of heteroatom nucleophiles,Pd-catalyzed difluoromethylation of arylboronic acids,and Cu-mediated trifluoromethylation of aryl iodides(via:CF_(2) and recombined CF_(3)-).These fluoroalkylation methods have been successfully applied to late-stage fluoroalkylation of drugs and drug-like molecules.

关键词： pentacoordinate phosphorane difluoromethyl radical difluorocarbene difluoromethylation fluoroalkylation

Rational modulation of electronic structure in PtAuCuNi alloys boosts efficient electrocatalytic ethanol oxidation assisted with energy-saving hydrogen evolution

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Journal of Energy chemistry 2024年第6期93卷 557-567,I0014页

作者： Hu Yao Yinan Zheng Xin Yu Songjie Hu Baolian Su Xiaohui Guo Key lab.of Synthetic and Natural Functional Molecule chemistry of Ministry of Education The College of Chemistry and Materials ScienceNorthwest UniversityXi’an 710069ShaanxiChina Department of Inorganic chemistry University of NamurBruxellesB-5000 NamurBelgium

Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient ***,we prepared a type of novel quaternary alloy catalyst(PtAuCuNi@NF)that exhibits excellent activity for EOR(0.215 V at 10 mA cm^(-2))and hydrogen evolution reaction(HER)(7 mV at 10 mA cm^(-2)).Experimental results demonstrated that both Cu and Ni modulated the electronic environment around Pt and *** electron-rich active center facilitates the rapid adsorption and dissociation of reactants and intermediates for both EOR and ***,in the ethanol-assisted overall water splitting(E-OWS),a current density of 10 mA cm^(-2)was achieved at 0.28 ***,an advanced acid-base self-powered system(A-Bsps)that can achieve a self-powered voltage of 0.59 V was ***,the self-driven hydrogen production with zero external power supply was realized by integrating A-Bsps with the E-OWS *** interesting results can provide a feasible strategy for designing and developing advanced nanoalloy-based materials for clean energy integration and use in various fields.

关键词： Pt-based alloy Electronic structure Ethanol oxidation Self-powered system Overall water splitting

Facile synthesis of hierarchical NiO/NiFe_(2)O_(4) microsphere composite as efficient visible photocatalyst for 2,4-DCP degradation

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Rare Metals 2024年第4期43卷 1580-1588页

作者： Shabana Shaheen Shuai Xu Ji Bian Amir Zada Zi-Qing Zhang Yang Qu Li-Qiang Jing Key lab.ratory of Functional Inorganic Materials chemistry(Ministry of Education) International Joint Research Center and Lab for Catalytic TechnologySchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin150080China Department of chemistry Abdul Wali Khan UniversityMardan23200Pakistan

It is highly desired to develop efficient photocatalysts with recycling property for practical application to degrade toxic ***,nanosheet-assembled NiFe_(2)O_(4)microspheres with commendable activity are successfully synthesized by a facile solvothermal reaction with NH4F as the modifier,and their photoactivities are further improved by coupling with NiO through an in situ growth *** optimized nickel oxide(NiO)/nickel ferrite(NiFe_(2)O_(4))microsphere composite(5NiO/NFO-4)exhibits a satisfactory photocatalytic activity for 2,4-dichlorophenol(2,4-DCP)degradation under visible-light irradiation,which is attributed to its wide visible-light response,well-designed hierarchical structure and enhanced charge transfer and separation by coupling NiO as a high-level energy platform to accept ***,it is found that the NiO/NiFe_(2)O_(4)microsphere photocatalysts can be easily collected and recycled owing to the distinctive magnetic *** work provides a feasible route to rational design visible-light-driven photocatalysts with high-activity for environmental remediation and purification with good recyclab.lity.

关键词： NiFe_(2)O_(4) microspheres NiO/Fe_(2)O_(4) composite Charge separation Visible-light photocatalysis 2 4-Dichlorophenol degradation

A highly sensitive multiple-mode optical thermometer designed in Eu^(2+)/^(3+)and Li^(+)co-doped polymorphism compound LaSc_(3)(BO_(3))_(4)

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Journal of Advanced Ceramics 2024年第6期13卷 821-833页

作者： Nan Yang Zhuo Li Tingxia Zhou Ziwang Zhang Wen Shi Yexiang Tong Jianxin Shi School of chemistry IGCMESun Yat-sen UniversityGuangzhou 510006China MOE of the Key lab.ratory of Bioinorganic and Synthetic chemistry IGCMEThe Key Lab of Low-Carbon Chemistry&Energy Conservation of Guangdong ProvinceSun Yat-sen UniversityGuangzhou 510006China

Noncontact optical thermometers have attracted widespread attention,but existing problems such as single-mode and low-sensitivity thermometers still urgently need to be ***,a novel multiple-mode thermometer was designed for the polymorphism LaSc_(3)(BO_(3))_(4):Eu^(2+/3+),Li^(+).X-ray diffraction(XRD)patterns revealed a slight transition betweenα-andβ-phases with the concentrations of the dopants,which is further proved by structure refinements and first-principles *** coexistence of Eu^(2+)and Eu^(3+)in the phosphors and their relative percentages were confirmed by X-ray absorption near-edge structure(XANES)*** from appropriate emissions from Eu^(2+)and Eu^(3+)without obvious energy transfer and their opposite changing trends with temperatures under 307 nm excitation,a triple-mode optical thermometer is obtained for this material within the temperature range of 150–450 *** highest sensitivities of 27.65,14.05,and 7.68%·K^(−1)are achieved based on two fluorescence intensity ratio(FIR)modes of Eu^(2+)and Eu^(3+)(5d–4f/^(5)D_(0)–^(7)F_(2,4))and the fluorescence lifetime(FL)mode of Eu^(2+),*** the best of our knowledge,the former is almost the highest in Eu^(2+)and Eu^(3+)co-doped *** results indicate that this material may be used as an excellent multiple-mode optical thermometer.

关键词： phase transition europium(Eu)ions multiple-mode optical thermometer thermal quenching properties fluorescence intensity ratio(FIR) fluorescence lifetime(FL)

Coupling Sb_(2)WO_(6)microflowers and conductive polypyrrole for efficient potassium storage by enhanced conductivity and K^(+) diffusivity

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Journal of Energy chemistry 2024年第2期89卷 250-258,I0007页

作者： Ruiqi Tian Hehe Zhang Zeyu Yuan Yuehua Man Jianlu Sun Jianchun Bao Ming-Sheng Wang Xiaosi Zhou School of chemistry and Materials Science Nanjing Normal UniversityNanjing 210023JiangsuChina State Key lab.of Physical chemistry of Solid Surfaces College of MaterialsXiamen UniversityXiamen 361005FujianChina

Although metal oxide compounds are considered as desirable anode materials for potassium-ion batteries(PIBs)due to their high theoretical capacity,the large volume variation remains a key issue in realizing metal oxide anodes with long cycle life and excellent rate *** this study,polypyrroleencapsulated Sb_(2)WO_(6)(denoted Sb_(2)WO_(6)@PPy)microflowers are synthesized by a one-step hydrothermal method followed by in-situ polymerization and coating by *** the nanosheet-stacked Sb_(2)WO_(6)microflower structure,the improved electronic conductivity,and the architectural protection offered by the PPy coating,Sb_(2)WO_(6)@PPy exhibits boosted potassium storage properties,thereby demonstrating an outstanding rate property of 110.3 m A h g^(-1)at 5 A g^(-1)and delivering a long-period cycling stability with a reversible capacity of 197.2 m A h g^(-1)after 500 cycles at 1 A g^(-1).In addition,the conversion and alloying processes of Sb_(2)WO_(6)@PPy in PIBs with the generation of intermediates,K_(2)WO_(4)and K_(3)Sb,is determined by X-ray photoelectron spectroscopy,transmission electron microscopy,and exsitu X-ray diffraction during potassiation/*** functional theory calculations demonstrate that the robust coupling between PPy and Sb_(2)WO_(6)endues it with a much stronger total density of states and a built-in electric field,thereby increasing the electronic conductivity,and thus effectively reduces the K^(+)diffusion barrier.

关键词： Sb_(2)WO_(6) Polypyrrole coating Anode Potassium-ion battery In-situ TEM observation

Construction of novel P-Si/TiO_(2)/HfO_(2)/MoS_(2)/Pt heterophotocathode for enhanced photoelectrochemical water splitting

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Nano Research 2024年第5期17卷 4428-4436页

作者： Jiaru Li Jiayu Bai Songjie Hu Wenyu Yuan Yuyu Bu Xiaohui Guo Key lab.of Synthetic and Natural Functional Molecule chemistry of Ministry of Education Shaanxi Key Laboratory for Carbon Neutral TechnologyThe College of Chemistry and Materials ScienceNorthwest UniversityXi'an 710069China Key lab.of Wide Band-Gap Semiconductor Materials and Devices School of MicroelectronicsXidian UniversityXi’an 710071China Key lab.of Macromolecular Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid ChemistryMinistry of EducationSchool of Chemistry&Chemical EngineeringShaanxi Normal UniversityXi'an 710062China

Photoelectrochemical devices have been developed to enable the conversion of solar ***,their commercial potential is restricted by the limited stability of the materials *** enhance the stability of photocathode and its solar water splitting performance,a P-Si/TiO_(2)/HfO_(2)/MoS_(2)/Pt composite photocathode is developed in this *** novel TiO_(2)/HfO_(2)/MoS_(2) serial nanostructure provides excellent stability of the photocathode,and optimizes the interface energy barrier to further facilitate the transfer process of photogenerated carriers within the *** best P-Si/TiO_(2)/HfO_(2)/MoS_(2)/Pt photocathode demonstrates an initial potential of 0.5 V(***)and a photocurrent density of-29 mA/cm^(2) at 0 V(***).Through intensity modulated photocurrent spectroscopy and photoluminescence test,it is known that the enhanced water splitting performance is attributed to the optimized carrier transfer *** findings provide a feasible strategy for the stability and photon quantum efficiency enhancement of silicon-based photocathode devices.

关键词： photoelectrochemical water splitting stability surface/interface engineering HfO_(2)layer