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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 laboratory of Molecule Synthesis and Function Discovery College of ChemistryFuzhou UniversityFuzhou 350108China state key laboratory of Organometallic chemistry and key laboratory 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 available diethyl bromodifluoromethanephosphonate(BrCF_(2)PO(OEt)_(2))as difluorocarbene precusor has been developed.This 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

The first chiral cerium halide towards circularly-polarized luminescence in the UV region

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Science China chemistry 2024年第6期67卷 1961-1968页

作者： Xinyi Niu Zhichao Zeng Zhaoyu Wang Haolin Lu Bing Sun Hao-Li Zhang Yongsheng Chen Yaping Du Guankui Long Tianjin key Lab for Rare Earth Materials and Applications Renewable Energy Conversion and Storage CenterSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin300350China Tianjin key Lab for Rare Earth Materials and Applications Center for Rare Earth and Inorganic Functional MaterialsHaihe Laboratory of Sustainable Chemical TransformationsSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin300350China state key laboratory of Applied organic chemistry Key Laboratory of Special Function Materials and Structure Design(Ministry of Education)College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000China The Centre of Nanoscale Science and Technology and state key laboratory of elemento-organic chemistry Frontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin300071China

Chiral organic-inorganic hybrid metal halides(OIHMHs)have attracted broader scientific community recently in spin lightemitting diodes,and circularly polarized light-emitting diodes.However,the emission peaks of the reported chiral OIHMHs mainly locate in the visible region,and chiral OIHMH with ultraviolet(UV)circularly polarized luminescence(CPL)has been rarely reported.To fill this gap,cerium,a unique rare-earth(RE)element with tunable luminescence from UV to the visible region owing to the 4 f-related electronic transition,was introduced to construct the first RE-based chiral OIHMHs,R/S-MCC.The chirality is successfully transferred from the chiral organic cations to the inorganic cerium chloride framework in R/S-MCC,as confirmed by the single crystal structures,circular dichroism,and CPL.The emission spectra of R/S-MCC are in the UV region,originating from the characteristic d-f transition of Ce^(3+),which making the Ce-based metal halides are ideal candidates towards CPL light sources in the UV region.Notably,R-and S-MCC are the first RE-based OIHMHs,also the first chiral metalhalides with UV CPL.Our work opens a new avenue for the development of the chiral OIHMH family towards RE-based chiral OIHMH.The RE-based chiral metal halides couple the unique and superior optical,electrical,magnetic,and spintronic properties of RE elements with chirality could accelerate the development of chiral optoelectronics and spintronics toward real applications.

关键词： chiral rare-earth halide ultraviolet circularly-polarized luminescence d-f transition rare-earth halide perovskite chiral perovskite

Atomic force microscopy-based nanoscale infrared techniques for liquid environments

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Science Bulletin 2024年第2期69卷 151-153页

作者： Jian Li Jing Liang Mu-Hao Lan Xing-Hua Xia state key laboratory of Analytical chemistry for Life Science School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Infrared(IR)light energy matches well with the vibration and rotation of chemical bonds in molecules,hence IR spectroscopy is commonly used for accurate molecular identification[1].Conventional IR analysis involves bulk samples,providing averaged information of the entire sample.The spatially-resolved investigation of heterogeneous sample properties is constrained by the micrometer-level spatial resolution of optical IR microscopy.

关键词： spatially hence rotation

Cobalt(III) hydride HAT mediated enantioselective intramolecular hydroamination access to chiral pyrrolidines

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Science China chemistry 2024年

作者： Qi Meng Tao Qin Huanran Miao Ge Zhang Qian Zhang state key laboratory of Organometallic chemistry Shanghai Institute of Organic Chemistry Chinese Academy of Sciences Jilin Province key laboratory of organic Functional Molecular Design & Synthesis Department of Chemistry Northeast Normal University

Enantioenriched pyrrolidines and derivatives are ubiquitous substructures in compounds of importance to medicinal and biological chemistry. Herein, we report an efficient cobalt-catalyzed intramolecular asymmetric hydroamination reaction that produces chiral pyrrolidines with good to excellent yield and enantiocontrol. Compared with previously reported radicalinvolved methodologies for enantioenriched pyrrolidines, these conditions feature two elegant versatilities, enabling(1) the use of cobalt-catalyzed hydrogen atom transfer(HAT) to generate organocobalt intermediates that bring radical reaction to organometallic chemistry, and(2) enantioselective intramolecular C–N bond forging through an SN2-like displacement involving dynamic kinetic resolution(DKR). This approach provides a new alternative and efficient methodology for enantioselective radical-involved C-N bond construction that can be used in the synthesis of both chiral pyrrolidines and homologous nitrogen heterocycles.

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Modularized viromimetic polymer nanoparticle vaccines(VPNVaxs) to elicit durable and effective humoral immune responses

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National Science Review 2024年第3期11卷 200-214页

作者： Zichao Huang Xinyu Zhuang Liping Liu Jiayu Zhao Sheng Ma Xinghui Si Zhenyi Zhu Fan Wu Ningyi Jin Mingyao Tian Wantong Song Xuesi Chen key laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of Sciences School of Applied chemistry and Engineering University of Science and Technology of China Changchun Veterinary Research Institute Chinese Academy of Agricultural Sciences Jilin Biomedical Polymers Engineering laboratory state key laboratory of Polymer Physics and chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

Virus-like particle(VLP) vaccines had shown great potential during the COVID-19 pandemic, and was thought to be the next generation of antiviral vaccine technology due to viromimetic structures. However,the time-consuming and complicated processes in establishing a current recombinant-protein–based VLP vaccine has limited its quick launch to the out-bursting pandemic. To simplify and optimize VLP vaccine design, we herein report a kind of viromimetic polymer nanoparticle vaccine(VPNVax), with subunit receptor-binding domain(RBD) proteins conjugated to the surface of polyethylene glycol-b-polylactic acid(PEG-b-PLA) nanoparticles for vaccination against SARS-CoV-2. The preparation of VPNVax based on synthetic polymer particle and chemical post-conjugation makes it possible to rapidly replace the antigens and construct matched vaccines at the emergence of different viruses. Using this modular preparation system, we identified that VPNVax with surface protein coverage of 20%–25% had the best immunostimulatory activity, which could keep high levels of specific antibody titers over 5 months and induce virus neutralizing activity when combined with an aluminum adjuvant. Moreover, the polymer nano-vectors could be armed with more immune-adjuvant functions by loading immunostimulant agents or chemical chirality design. This VPNVax platform provides a novel kind of rapidly producing and efficient vaccine against different variants of SARS-CoV-2 as well as other viral pandemics.

关键词： vaccine polymer nanomaterials SARS-CoV-2

Electrochemical synthesis of trimetallic nickel-iron-copper nanoparticles via potential-cycling for high current density anion exchange membrane water-splitting applications

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Journal of Energy chemistry 2024年第2期89卷 535-542,I0012页

作者： Ziqi Zhang Sheng Wan Hanbo Wang Jinghan He Ruige Zhang Yuhang Qi Haiyan Lu state key laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012JilinChina

Hydrogen is known for its elevated energy density and environmental compatibility and is a promising alternative to fossil fuels.Alkaline water electrolysis utilizing renewable energy sources has emerged as a means to obtain high-purity hydrogen.Nevertheless,electrocatalysts used in the process are fabricated using conventional wet chemical synthesis methods,such as sol-gel,hydrothermal,or surfactantassisted approaches,which often necessitate intricate pretreatment procedures and are vulnerable to post-treatment contamination.Therefore,this study introduces a streamlined and environmentally conscious one-step potential-cycling approach to generate a highly efficient trimetallic nickel-iron-copper electrocatalyst in situ on nickel foam.The synthesized material exhibited remarkable performance,requiring a mere 476 mV to drive electrochemical water splitting at 100 mA cm^(-2)current density in alkaline solution.Furthermore,this material was integrated into an anion exchange membrane watersplitting device and achieved an exceptionally high current density of 1 A cm^(-2)at a low cell voltage of2.13 V,outperforming the noble-metal benchmark(2.51 V).Additionally,ex situ characterizations were employed to detect transformations in the active sites during the catalytic process,revealing the structural transformations and providing inspiration for further design of electrocatalysts.

关键词： Electrocatalytic water splitting Hydrogen evolution reaction Oxygen evolution reaction Electrochemical synthesis Anion exchange membrane

Multifunctional dual-anion compensation of amphoteric glycine hydrochloride enabled highly stable perovskite solar cells with prolonged carrier lifetime

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Nano Research 2024年第6期17卷 5131-5137页

作者： Lina Qin Mengfei Zhu Yuren Xia Xingkai Ma Daocheng Hong Yuxi Tian Zuoxiu Tie Zhong Jin state key laboratory of Coordination chemistry MOE Key Laboratory of Mesoscopic ChemistryMOE Key Laboratory of High Performance Polymer Materials and TechnologyJiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Nanjing Tieming Energy Technology Co.Ltd. Nanjing 210093China Suzhou Tierui New Energy Technology Co.Ltd. Suzhou 215228China

Throughout years,the two-step spin-coating process is the most common method to prepare organic lead halide perovskite materials.However,the short reaction time of dropping the solution at the second step means that PbI2 cannot be completely transformed into perovskite phase.To solve this problem,we report the introduction of glycine hydrochloride(GlyHCl)into the second step of the two-step spin-coating process to prepare a FA_(0.9)MA_(0.1)PbI_(3-x)%-GlyHCl perovskite material(namely FAMA-x%-GlyHCl,where FA=formamidinium,MA=methylammonium,and x%stands for the molar ratio of GlyHCl added in FA iodide/MA iodide(FAI/MAI)precursor solution).The Cl−ion in GlyHCl assists the formation ofα-phase perovskite,and the-COO−group coordinates with Pb2+cation in a bridging way,making up for the anion vacancy in perovskite lattice and resulting in high absorption intensity.The perovskite solar cells(PSCs)based on FAMA-9%-GlyHCl achieve a long carrier lifetime(527.0 ns),a photoelectric conversion efficiency(PCE)of 19.40%and good thermal stability,maintaining 85.8%of the initial PCE after being continuously heated at 60℃for 500 h.This study helps to solve the problem of incomplete reaction in the two-step spin-coating process and puts forward a new solution for preparing high coverage perovskite films with large grain size.

关键词： dual-anion compensation glycine hydrochloride perovskite solar cells carrier lifetime thermal and moisture stability

In-situ synthesis of quantum dots in the nucleus of live cells

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National Science Review 2024年第3期11卷 172-182页

作者： Yusi Hu Zhi-Gang Wang Haohao Fu Chuanzheng Zhou Wensheng Cai Xueguang Shao Shu-Lin Liu Dai-Wen Pang state key laboratory of Medicinal Chemical Biology Frontiers Science Centre for New Organic MatterTianjin Key Laboratory of Biosensing and Molecular Recognition Research Centre for Analytical Sciences College of Chemistry School of Medicine and Frontiers Science Centre for Cell Responses Nankai University Haihe laboratory of Sustainable Chemical Transformations

The cell nucleus is the main site for the storage and replication of genetic material, and the synthesis of substances in the nucleus is rhythmic, regular and strictly regulated by physiological processes. However,whether exogenous substances, such as nanoparticles, can be synthesized in situ in the nucleus of live cells has not been reported. Here, we have achieved in-situ synthesis of CdSxSe1-xquantum dots（QDs） in the nucleus by regulation of the glutathione（GSH） metabolic pathway. High enrichment of GSH in the nucleus can be accomplished by the addition of GSH with the help of the Bcl-2 protein. Then, high-valence Se is reduced to low-valence Se by glutathione-reductase-catalyzed GSH, and interacts with the Cd precursor formed through Cd and thiol-rich proteins, eventually generating QDs in the nucleus. Our work contributes to a new understanding of the syntheses of substances in the cell nucleus and will pave the way for the development of advanced ‘supercells’.

关键词： glutathione live cell nucleus quantum dot intracellular synthesis

Highly selective photocatalytic reduction of CO_(2) to CH_(4) on electron-rich Fe species cocatalyst under visible light irradiation

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Carbon Energy 2024年第1期6卷 255-266页

作者： Qianying Lin Jiwu Zhao Pu Zhang Shuo Wang Ying Wang Zizhong Zhang Na Wen Zhengxin Ding Rusheng Yuan Xuxu Wang Jinlin Long state key laboratory of Photocatalysis on Energy and Environment College of ChemistryFuzhou UniversityFuzhouChina

Efficient photocatalytic reduction of CO_(2) to high-calorific-value CH4,an ideal target product,is a blueprint for C_(1)industry relevance and carbon neutrality,but it also faces great challenges.Herein,we demonstrate unprecedented hybrid SiC photocatalysts modified by Fe-based cocatalyst,which are prepared via a facile impregnation-reduction method,featuring an optimized local electronic structure.It exhibits a superior photocatalytic carbon-based products yield of 30.0μmol g^(−1) h^(−1) and achieves a record CH_(4) selectivity of up to 94.3%,which highlights the effectiveness of electron-rich Fe cocatalyst for boosting photocatalytic performance and selectivity.Specifically,the synergistic effects of directional migration of photogenerated electrons and strongπ-back bonding on low-valence Fe effectively strengthen the adsorption and activation of reactants and intermediates in the CO_(2)→CH_(4) pathway.This study inspires an effective strategy for enhancing the multielectron reduction capacity of semiconductor photocatalysts with low-cost Fe instead of noble metals as cocatalysts.

关键词： artificial synthesis of CH_(4) electronic structure optimization Fe species cocatalyst photocatalytic CO_(2) reduction SiC

S-(1,3-Dioxoisoindolin-2-yl)O,O-diethyl phosphorothioate (SDDP): A practical electrophilic reagent for the phosphorothiolation of electron-rich compounds

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Chinese Chemical Letters 2024年第5期35卷 151-154页

作者： Ze-Yuan Ma Mei Xiao Cheng-Kun Li Adedamola Shoberu Jian-Ping Zou key laboratory of organic Synthesis of Jiangsu Province College of Chemistry and Chemical EngineeringSoochow UniversitySuzhou 215123China

An efficient synthesis of the electrophilic reagent,S-(1,3-dioxoisoindolin-2-yl)O,O-diethyl phosphorothioate(SDDP)is described.Moreover,the synthetic applications of SDDP wherein the transfer of the SP(O)(OEt)_(2) moiety occurs were investigated.In this manner,SDDP underwent facile SP(O)(OEt)_(2) transfer with electron-rich substrates such as ketones,indoles,and thiols to formα-phosphorothiolated ketones,3-phosphorothiolated indoles and S-phosphorothiolated thioethers,respectively.

关键词： Electrophilic reagent Phosphorothiolation Electrophilic substitution