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Electrochemical Reduction of Benzo[b]thiophene 1,1-Dioxides with HFIP as Hydrogen Donor

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Chinese Journal of chemistry 2024年第6期42卷 585-591页

作者： Ming-Zhong Guo Mei-Jin Mou Zhuo Chen Shao-Fei Ni Ming Li Li-Rong Wen Lin-Bao Zhang State key laboratory Base of Eco-Chemical Engineering College of Chemistry and Molecular EngineeringQingdao University of Science & TechnologyQingdaoShandong266042 China department of chemistry and key laboratory for preparation and application of ordered structural Materials of Guangdong Province Shantou UniversityShantouGuangdong515063 China

A straightforward electrochemical reduction of benzo[b]thiophene 1,1-dioxides with HFIP as the hydrogen donor has been reported in an undivided cell under metal-free ***,the tolerance of various functional groups and ... 详细信息

关键词： Electrochemistry Reduction Benzo[b]thiophene 1,1-dioxides Deuterium Hydrogen source

Bioinspired zinc-mediated umpolung thiolation of alkyl electrophiles: reaction development, scope and mechanism

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Science China chemistry 2024年第3期67卷 898-907页

作者： Yuenian Xu Yan Zhang Yong Liu Wen-Wu Sun Jie Huang Hui He Yingjie Wu Wen Liu Shao-Fei Ni Xu-Qiong Xiao Xinxin Shao College of Material Chemistry and Chemical EngineeringKey Laboratory of Organosilicon Chemistry and Material Technology of Ministry of EducationHangzhou Normal UniversityHangzhou 311121China School of Pharmaceutical Sciences South-Central Minzu UniversityWuhan 430074China department of chemistry and key laboratory for preparation and application of ordered structural Materials of Guang-dong Province Shantou UniversityShantou 515063China

Zinc-promoted umpolung thiolation of alkyl electrophiles with masked sulfur transfer reagents in the absence of nickel or copper catalysis is described. This protocol proceeds via a SET process of Zn to electrophilic sulfur reagent followed by insertion of Zn into disulfide and nucleophilic thiolation, providing straightforward access to a wide range of alkyl sulfides with broad substrate scope. A neutral TMEDA-ligated four-coordinated zinc thiolate with tetrahedra geometry was synthesized, isolated and fully characterized by NMR, IR and X-ray analysis. More importantly, the chemical reactivity of this active intermediate has been investigated, enabling the construction of C-Se, C-Te, Sb-S and Bi-S bonds to prepare valuable sulfur-containing molecules and beyond.

关键词： umpolung thiolation C(sp^(3))-S bond formation masked sulfur reagents reductive coupling

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Producing circularly polarized luminescence by radiative energy transfer from achiral metal-organic cage to chiral organic molecules

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Chinese Chemical Letters 2024年第8期35卷 498-502页

作者： Zhao-Xia Lian Xue-Zhi Wang Chuang-Wei Zhou Jiayu Li Ming-De Li Xiao-Ping Zhou Dan Li College of chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China College of chemistry and Chemical Engineering Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong ProvinceShantou UniversityShantou 515063China

The development of circularly polarized luminescence(CPL)materials with high performance is signifi-cantly ***,we develop a facial strategy for fabricating a CPL-active system by employing an achiral luminescent metal-organic cage(MOC)and chiral boron dipyrromethene(BODIPY)*** is achieved by taking advantage of the radiative energy transfer process,in which BODIPY molecules act as energy acceptors and MOCs act as *** CPL performance(maximum luminescence dissymme-try factor up to±1.5×10^(−3))can be tuned by adjusting the ratio between MOCs and ***-light emission with the CPL feature is obtained by using a ternary system including MOC,chiral BODIPY,and Rhodamine *** present work provides a facile and universal strategy to construct a CPL-active system by integrating achiral luminophores and chiral molecules.

关键词： Circularly polarized luminescence Metal-organic cage Radiative energy transfer Chiral small molecules Bodipy Chirality

A strained π-extended[10]cycloparaphenylene carbon nanoring

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Chinese Chemical Letters 2024年第5期35卷 171-174页

作者： Kang Wei Jiayu Li Wen Zhang Bing Yuan Ming-De Li Pingwu Du key laboratory of Precision and Intelligent chemistry Anhui Laboratory of Advanced Photon Science and TechnologyDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China department of chemistry and key laboratory for preparation and application of ordered structural Materials of Guangdong Province Shantou UniversityShantou 515063China

Herein,we report the facile synthesis of a highly strained hexabenzocoronene-containing carbon nanoring,cyclo[4]-paraphenylene[2]-2,11-hexabenzocoronenylene([4,2]CPHBC),as the segment of a[10,10]single-walled carbon nanotube([10,10]SWNT).[4,2]CPHBC was synthesized based on the platinummediated assembly of diborylbiphenyl and diborylhexabenzocoronene,forming a tetranuclear platinum complex,followed by reductive *** nanoring molecule was confirmed by NMR and HRMS,and its photophysical properties were studied using steady-state and time-resolved ***,the selective supramolecular host-guest interaction between[4,2]CPHBC and C_(60) was also investigated.

关键词： CPP Hexabenzocoronene Fullerene Supramolecular chemistry

Chemoselective electrochemical seleno-cyclization of dienes to medium-sized benzo[b]azocines

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Chinese Chemical Letters 2024年第2期35卷 431-435页

作者： Zhichuan Wang Xin Wang Quanxin Li Shaofei Ni Dongyang Zhao Shubin Yang Ge Qiu Kai Sun College of chemistry and Chemical Engineering Yantai UniversityYantai 264005China department of chemistry and key laboratory for preparation and application of ordered structural Materials of Guangdong Province Shantou UniversityShantou 515063China Aix Marseille Univ. CNRSCentrale MarseilleiSm2MarseilleFrance

The preparation of medium-sized benzo[b]azocines has always been challenging because of inherently unfavorable enthalpy and entropy *** report presents a novel approach for accessing 8-membered seleno-benzo[b]azocines via electrochemically-driven *** method enables room-temperature preparation of various structurally diverse medium-sized seleno-benzo[b]*** facile deselenation of the seleno-cyclization products to generate functionalized dienes is an additional benefit of this indispensable *** insights are presented based on radical inhibition experiments and cyclic voltammetry measurements,which elucidate the radical ***,density functional theory calculations further rationalize the rate-determining step and the unique chemoselectivity observed in this transformation.

关键词： Medium-sized n-heterocycles Electrocatalysis Radical Mechanistic insights Selenylation

Luminescence regulation of Sb^(3+)in 0D hybrid metal halides by hydrogen bond network for optical anti-counterfeiting

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Opto-Electronic Advances 2024年第3期7卷 15-25页

作者： Dehai Liang Saif M.H.Qaid Xin Yang Shuangyi Zhao Binbin Luo Wensi Cai Qingkai Qian Zhigang Zang key laboratory of Optoelectronic Technology&Systems(Ministry of Education) Chongqing UniversityChongqing 400044China department of Physics&Astronomy College of SciencesKing Saud UniversityP.O.Box 2455Riyadh 11451Saudi Arabia department of chemistry and Chemical Engineering Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong ProvinceShantou UniversityShantou 515063China department of Oil Army Logistics Academy of PLAChongqing 401311China

The Sb^(3+) doping strategy has been proven to be an effective way to regulate the band gap and improve the photophysical properties of organic-inorganic hybrid metal halides(OIHMHs).However,the emission of Sb^(3+) ions in OIHMHs is primarily confined to the low energy region,resulting in yellow or red *** date,there are few reports about green emission of Sb^(3+)-doped ***,we present a novel approach for regulating the luminescence of Sb^(3+) ions in 0D C_(10)H_(2)_(2)N_(6)InCl_(7)·H_(2)O via hydrogen bond network,in which water molecules act as agents for hydrogen ***^(3+)-doped C_(10)H_(2)2N_(6)InCl_(7)·H_(2)O shows a broadband green emission peaking at 540 nm and a high photoluminescence quantum yield(PLQY)of 80%.It is found that the intense green emission stems from the radiative recombination of the self-trapped excitons(STEs).Upon removal of water molecules with heat,C_(10)H_(2)_(2)N_(6)In_(1-x)Sb_(x)Cl_(7) generates yellow emis-sion,attributed to the breaking of the hydrogen bond network and large structural distortions of excited *** water molecules are adsorbed by C_(10)H_(2)_(2)N_(6)In_(1-x)Sb_(x)Cl_(7),it can subsequently emit green *** water-induced reversible emission switching is successfully used for optical security and information *** findings expand the under-standing of how the local coordination structure influences the photophysical mechanism in Sb^(3+)-doped metal halides and provide a novel method to control the STEs emission.

关键词： indium-based halides Sb^(3+)doping hydrogen bonding network optical anti-counterfeiting

Intense Intramolecular Charge Transfer Endows Cyanated Polymer with Broad Absorption,Intensified Light-Harvesting,Long-Lived Exciton,and Superior Photovoltaic Property

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CCS chemistry 2024年第9期6卷 2318-2332页

作者： Jinming Chen Huijuan Wang Songmin Mo Hui Chen Xinyu He Mingbin Su Dongyan Li Yonghong Xiao Zhiqi Wang Fanwei Ye Mingde Li Li Dang Xiao-Chun Huang Chang-Zhi Li Feng He Qinghe Wu key laboratory for preparation and application of ordered structural Materials of Guangdong Department of ChemistryShantou UniversityShantou 515063 department of chemistry Shenzhen Grubbs InstituteSouthern University of Science and TechnologyShenzhen 518055 department of Polymer Science and Engineering Zhejiang UniversityHangzhou 310027 chemistry and Chemical Engineering Guangdong laboratory Shantou 515063 Guangdong Provincial key laboratory of Catalysis Southern University of Science and TechnologyShenzhen 518055

The donor–acceptor(D–A)copolymers,which exhibit wide broad absorption and intensified light-harvesting,are highly captivating for applications in solar conversion and ***,designing a polymer structure that can achieve these photophysical properties simultaneously remains a ***,we report two novel cyanated units 4-cyanobenzo[1,2-b:6,5-b′:3,4-c″]trithiophene(CBT)and 4,6-dicyanobenzo[1,2-b:6,5-b′:3,4-c″]trithiophene(C2BT)and their corresponding polymers,PCBT and *** interestingly,the PC2BT exhibited a broad absorption band with full width at half maxima(FWHM)of its absorption spectra,almost twice wider than PCBT and benchmark polymers PM6 and ***,the PC2BT demonstrated intensified light-harvesting and long-lived *** in-depth investigation unveiled that the presence of dicyano substitutions induced a strong intramolecular charge transfer(ICT),which,in turn,resulted in the formation of favorable photophysical ***,PC2BT-based polymer solar cells(PSCs)exhibited an efficiency of 18.06%,which was a record-setting efficiency for cyanated *** study suggests an efficient strategy for enhancing ICT to design polymers toward favorable photophysical properties and excellent photovoltaic performance.

关键词： intramolecular charge transfer broad absorption band dicyanobenzotrithiophene cyanated polymer polymer solar cell

Organic stoichiometric cocrystals with a subtle balance of charge-transfer degree and molecular stacking towards high-efficiency NIR photothermal conversion

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Chinese Chemical Letters 2024年第10期35卷 180-186页

作者： Jieqiong Xu Wenbin Chen Shengkai Li Qian Chen Tao Wang Yadong Shi Shengyong Deng Mingde Li Peifa Wei Zhuo Chen Institutes of Physical Science and Information Technology Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationAnhui Graphene Engineering LaboratoryAnhui UniversityHefei 230601China Molecular Science and Biomedicine laboratory(MBL).State key laboratory of Chemo/Biosensing and Chemometrics College of Chemistry and Chemical EngineeringCollege of BiologyAptamer Engineering Center of Hunan ProvinceHunan UniversityChangsha 410082China department of chemistry and key laboratory for preparation and application of ordered structural Materials of Guangdong Province Shantou UniversityShantou515063China

Charge-transfer(CT)stoichiometric cocrystals are promising choice of organic materials for unveiling the structure-property ***,due to the contradiction between large CT degree required for strong NIR absorption and flexible molecular stacking,construction of stoichiomorphism-based cocystals with near-infrared(NIR)photothermal property remains ***,the first example of stoichiomorphism-based photothermal cocrystals were accomplished through the adaptive assembly of 3,3,5,5-tetramethylbenzidine(TMB)donor and 1,2,4,5-tetracyanobenzene(TCNB)*** selective cocrystallization could be controlled by varying the donor-acceptor stoichiometries via a surfactantassisted method,resulting in two cocrystals with 1:1(T1C1)and 1:2(T2C1)*** absorbance intensity of T1C1 at 808 nm was nearly twice that of T2C1,while the photothermal conversion efficiency(PCE)of the former was 60.3%±0.6%,approximately 80%of that for the latter(75.5%±2.6%),which might be caused by the different intermolecular interactions in distinct molecular stacking ***,both excellent PCEs of stoichiometric cocrystals were attributed to the nonradiative transition process,including internal conversion and charge dissociation processes,as elucidated by femtosecond transient absorption spectroscopy ***,T1C1 was used as an NIR heater for preparing agarose-based photothermal hydrogel,showing great potential for light-controlled in-situ *** strategy of balancing the CT degree and molecular packing orientation not only uncovered the relationship between stoichiometric stacking and photothermal property,but also provided an opportunity to develop advanced organic optoelectronic materials.

关键词： Charge-transfer cocrystal Stoichiometric stacking Crystal growth Photothermal conversion In-situ gelation

Insights into ionic association boosting water oxidation activity and dynamic stability

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Journal of Energy chemistry 2024年第2期89卷 99-109,I0004页

作者： Zanling Huang Shuqi Zhu Yuan Duan Chaoran Pi Xuming Zhang Abebe Reda Woldu Jing-Xin Jian Paul K.Chu Qing-Xiao Tong Liangsheng Hu Xiangdong Yao department of chemistry and key laboratory for preparation and application of ordered structural Materials of Guangdong Province Shantou UniversityShantou 515063GuangdongChina chemistry and Chemical Engineering Guangdong laboratory Shantou 515063GuangdongChina State key laboratory of Refractories and Metallurgy and Institute of Advanced Materials and Nanotechnology Wuhan University of Science and TechnologyWuhan 430081HubeiChina department of Physics Department of Materials Science and Engineeringand Department of Biomedical EngineeringCity University of Hong KongTat Chee AvenueKowloonHong KongChina School of Advanced Energy Sun Yat-sen University(Shenzhen)Shenzhen 518107GuangdongChina

There have been reports about Fe ions boosting oxygen evolution reaction(OER)activity of Ni-based catalysts in alkaline conditions,while the origin and reason for the enhancement remains ***,we attempt to identify the activity improvement and discover that Ni sites act as a host to attract Fe(Ⅲ)to form Fe(Ni)(Ⅲ)binary centres,which serve as the dynamic sites to promote OER activity and stability by cyclical formation of intermediates(Fe(Ⅲ)→Fe(Ni)(Ⅲ)→Fe(Ni)-OH→Fe(Ni)-O→Fe(Ni)OOH→Fe(Ⅲ))at the electrode/electrolyte interface to emit O_(2).Additionally,some ions(Co(Ⅱ),Ni(Ⅱ),and Cr(Ⅲ))can also be the active sites to catalyze the OER process on a variety of *** Fe(Ⅲ)-catalyzed overall water-splitting electrolyzer comprising bare Ni foam as the anode and Pt/Ni-Mo as the cathode demonstrates robust stability for 1600 h at 1000 mA cm^(-2)@~1.75 *** results provide insights into the ioncatalyzed effects boosting OER performance.

关键词： Oxygen evolution reaction Fe(Ⅲ)-catalysis Ni-Fe binary active centers Ion-catalyzed effects Robust stability