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Total synthesis of Laurane and Guaiane Sesquiterpenoids via Oxidative Nazarov Reaction

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Chinese Journal of Chemistry 2024年第11期42卷 1267-1274页

作者： Yuye Chen Wenqing Chen Zhiting Zhang Jing Xu Shenzhen Grubbs Institute and Department of Chemistry and Guangming Advanced Research Institute and Guangdong Provincial Key laboratory of Catalysis and Shenzhen Key laboratory of Small Molecule Drug Discovery and synthesis Southern University of Science and TechnologyShenzhenGuangdong518055 China

As one of the most common structural motifs in natural products,cyclopentenones usually can be fabricated by Nazarov cyclization using divinyl ketones or functionalized tertiary divinyl carbinols(TDCs)as ***,straightforward method for transforming unfunctionalized TDCs to their corresponding cyclopentenones is currently ***,we wish to report the total syntheses of four structurally distinct terpenoids,namely laurane-type marine sesquiterpenoids isolaurene,debromoaplysin and aplysin,and guaiane sesquiterpenoid guaiadienone A,all using a novel synthetic method,named oxidative Nazarov cyclization,as the key *** work demonstrated our robust method is suitable for synthesizing various highly substituted cyclopentenones.

关键词： Total synthesis Synthetic methods Sesquiterpenoids Oxidative Nazarov reaction Electrocyclization Oxoammonium salt Pericyclic reaction Annulation

Tailoring component incorporation for homogenized perovskite solar cells

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Science Bulletin 2024年第16期69卷 2555-2564页

作者： Wenhan Yang Junmin Xia Yuexin Lin Hao Gu Fengqiang Ma Yumin Ren Fenqi Du Dejian Yu Jinfeng Liao Yiwang Chen Guojia Fang Shengchun Yang Chao Liang MOE Key laboratory for Nonequilibrium synthesis and Modulation of Condensed Matter School of PhysicsNational Innovation Platform(Center)for Industry-Education Integration of Energy Storage TechnologyXi’an Jiaotong UniversityXi’an 710049China State Key laboratory of organic Electronics and Information Displays&Institute of Advanced Materials(IAM) Nanjing University of Posts&TelecommunicationsNanjing 210023China Joint Key laboratory of the Ministry of Education Institute of Applied Physics and Materials EngineeringUniversity of MacaoMacao 999078China Shandong Zhixin Intelligent Equipment Co. LTDJinan 250101China School of Chemistry Xi’an Jiaotong UniversityXi’an 710049China National Engineering Research Center for Carbohydrate synthesis Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of EducationJiangxi Normal UniversityNanchang 330022China Key laboratory of Artificial Micro/Nano Structures of Ministry of Education School of Physics and TechnologyWuhan UniversityWuhan 430072China

Deep-level traps at the buried interface of perovskite and energy mismatch problems between the perovskite layer and heterogeneous interfaces restrict the development of ideal homogenized films and efficient perovskite solar cells(PSCs)using the one-step spin-coating ***,we strategically employed sparingly soluble germanium iodide as a homogenized bulk in-situ reconstruction inducing material preferentially aggregated at the perovskite buried interface with gradient doping,markedly reducing deep-level traps and withstanding local lattice strain,while minimizing non-radiative recombination losses and enhancing the charge carrier lifetime over 9μ***,this gradient doping assisted in modifying the band diagram at the buried interface into a desirable flattened alignment,substantially mitigating the energy loss of charge carriers within perovskite films and improving the carrier extraction *** a result,the optimized device achieved a champion power conversion efficiency of 25.24% with a fill factor of up to 84.65%,and the unencapsulated device also demonstrated excellent light stability and humidity *** work provides a straightforward and reliable homogenization strategy of perovskite components for obtaining efficient and stable PSCs.

关键词： Homogenized perovskite films Lattice strain relaxation Deep-level traps Carrier extraction equilibrium Perovskite solar cells

Recent advances in the synthesis and application of N-heterocyclic carbene-based molecular cages

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Science China Chemistry 2024年第5期67卷 1510-1523页

作者： Qiongjie Chai Lixin Duan Yanzhe Ma Tianheng Hou Tao Tu Shanghai Key laboratory of Molecular Catalysis and Innovative Materials Department of ChemistryFudan UniversityShanghai 200438China State Key laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

N-Heterocyclic carbene(NHC)-based cages have emerged as a prominent and dynamic research area within the research field of chemistry. Leveraging the distinctive electronic and steric properties of NHC ligands, the design, synthesis, and application of these corresponding cages have garnered substantial scholarly interest. In recent years, we have witnessed the successful fabrication of diverse NHC-based cages through a range of synthetic methodologies, which hold significant potential for applications in molecular recognition and catalysis. In this review, we delve into the foundational synthetic strategies that underlie the creation of NHC-based cages, employing approaches encompassing metal–NHC chelation, coordination assembly,and covalent bonding. Additionally, we compile the diverse applications of these cages within catalytic processes and molecular recognition. Lastly, we shed light on the current limitations of synthesis and outline future trends in the development of NHCbased cages.

关键词： N-heterocyclic carbene molecular cages supramolecular chemistry synthetic strategies applications

Function-reversible facets enabling SrTiO_(3)nanocrystals for improved photocatalytic hydrogen evolution

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Frontiers in Energy 2024年第1期18卷 101-109页

作者： Bin WANG Bei AN Xiaoqian LI Shaohua SHEN School of Physics Key Laboratory for Non-equilibrium Synthesis and Modulation of Condensed Matter(Ministry of Education)Key Laboratory of Shaanxi for Advanced Materials and Mesoscopic PhysicsXi’an Jiaotong UniversityXi’an 710049China International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power EngineeringXi’an Jiaotong UniversityXi’an 710049China

It has been widely reported that,for faceted nanocrystals,the two adjacent facets with different band levels contribute to promoted charge separation,and provide active sites for photocatalytic reduction and oxidation reaction,*** such cases,only one family of facets can be used for photocatalytic hydrogen ***,by using SrTiO_(3)nanocrystals enclosed by{023}and{001}facets as a model photocatalyst,this paper proposed a strategy to achieve the full-facets-utilization of the nanocrystals for photocatalytic hydrogen via chemically depositing Pt nanoparticles on all *** photo-deposition experiment of CdS provided direct evidence to demonstrate that the{023}facets which were responsible for photooxidation reaction can be function-reversed for photocatalytic hydrogen evolution after depositing Pt nanoparticles,together with the{001}***,the full-facets-utilization led to a much-improved activity for photocatalytic hydrogen,in contrast to those SrTiO_(3)nanocrystals with only{001}facets deposited by Pt nanoparticles via a photo-deposition method.

关键词： SrTiO_(3)nanocrystals crystal facets photocatalysis hydrogen evolution

One-shot synthesis of heavy-atom-modified carbazole-fused multi-resonance thermally activated delayed fluorescence materials

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Science China Materials 2024年第9期67卷 2789-2795页

作者： Jia-Jun Hu Jia-Qi Liang Zhi-Ping Yan Hua-Xiu Ni Xiang-Ji Liao You-Xuan Zheng State Key laboratory of Coordination Chemistry Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing210023China Green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou450001China

Efficient multi-resonance thermally activated delayed fluorescence(MR-TADF)materials hold significant potential for applications in organic light-emitting diodes(OLEDs)and ultra-high-definition ***,the stringent synthesis conditions and low yields typically associated with these materials pose substantial challenges for their practical *** this study,we introduce an innovative strategy that involves peripheral modification with sulfur and selenium atoms for two materials,CFDBNS and *** approach enables a directed one-shot borylation process,achieving synthesis yields of 66%and 25%,respectively,while also enhancing reverse intersystem crossing *** emitters exhibit ultra-narrowband sky-blue emissions centered around 474 nm,with full width at half maximum(FWHM)values as narrow as 19 nm in dilute toluene solutions,along with high photoluminescence quantum yields of 98%and 99%in doped films,*** OLEDs based on CFDBNS and CFDBNSe display sky-blue emissions with peaks at 476 and 477 nm and exceptionally slender FWHM values of 23 ***,the devices demonstrate remarkable performances,achieving maximum external quantum efficiencies of 24.1%and 27.2%.This work presents a novel and straightforward approach for the incorporation of heavy atoms,facilitating the rapid construction of efficient MR-TADF materials for OLEDs.

关键词： one-shot synthesis multi-resonance thermally activated delayed fluorescence carbazole-fused dual-boron embedded framework ultra-narrowband emission organic light-emitting diode

Optimizing magnetoelastic properties by machine learning and high-throughput micromagnetic simulation

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Rare Metals 2024年第5期43卷 2251-2262页

作者： Jian-Hu Gong Zheng-Ming Zhang Cheng-Liang Zhang Peng-Qiang Hu Chao Zhou Dun-Hui Wang Sen Yang Division of Microelectronic Materials and Devices Hangzhou Dianzi UniversityHangzhou 310018China School of Physics MOEKey Laboratory forNonequilibrium Synthesis and Modulation of Condensed Matter and State Key Laboratory for Mechanical Behavior of MaterialsXi'an Jiaotong UniversityXi'an 710049China National laboratory of Solid State Microstructures Nanjing UniversityNanjing210093China

Magnetoelastic couplings in giant magnetostrictive materials(GMMs)attract significant interests due to their extensive applications in the fields of spintronics and energy harvesting *** the role of the selection of materials and the response to external fields is essential for attaining desired functionality of a ***,machine learning(ML)models are conducted to predict saturation magnetostrictions(λ_(s))in RFe_(2)-type(R=rare earth)GMMs with different *** to ML-predicted composition–λsrelations,it is discovered that the values ofλshigher than1100×10^(-6)are almost situated in the composition space surrounded by 0.26≤x≤0.60 and 1.90≤y≤2.00 for the ternary compounds of Tb_(x)Dy_(1-x)Fe_(y).Assisted by ML predictions,the compositions are further narrowed down to the space surrounded by 0.26≤x≤0.32 and 1.92≤y≤1.97 for the excellent piezomagnetic(PM)performance in the Tb_(x)Dy_(1-x)Fe_(y)based PM device through our developed high-throughput(HTP)micromagnetic simulation(MMS)***,high sensitivities up to10.22-13.61 m T·MPa^(-1)are observed in the optimized range within which the available experimental data fall *** work not only provides valuable insights toward understanding the mechanism of magnetoelastic couplings,but also paves the way for designing and optimizing highperformance magnetostrictive materials and PM sensing devices.

关键词： Magnetostriction Piezomagnetic effect Machine learning Micromagnetic simulation

Flexible and Robust Functionalized Boron Nitride/Poly(p‑Phenylene Benzobisoxazole)Nanocomposite Paper with High Thermal Conductivity and Outstanding Electrical Insulation

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Nano-Micro Letters 2024年第2期16卷 423-437页

作者： Lin Tang Kunpeng Ruan Xi Liu Yusheng Tang Yali Zhang Junwei Gu Chongqing Key laboratory of Green synthesis and Applications College of ChemistryChongqing Normal UniversityChongqing 401331People’s Republic of China Shaanxi Key laboratory of Macromolecular Science and Technology School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an 710072People’s Republic of China

With the rapid development of 5G information technology,thermal conductivity/dissipation problems of highly integrated electronic devices and electrical equipment are becoming *** this work,“high-temperature solid-phase&diazonium salt decomposition”method is carried out to prepare benzidine-functionalized boron nitride(m-BN).Subsequently,m-BN/poly(pphenylene benzobisoxazole)nanofiber(PNF)nanocomposite paper with nacremimetic layered structures is prepared via sol–gel film transformation *** obtained m-BN/PNF nanocomposite paper with 50 wt%m-BN presents excellent thermal conductivity,incredible electrical insulation,outstanding mechanical properties and thermal stability,due to the construction of extensive hydrogen bonds andπ–πinteractions between m-BN and PNF,and stable nacre-mimetic layered ***λ∥andλ_(⊥)are 9.68 and 0.84 W m^(-1)K^(-1),and the volume resistivity and breakdown strength are as high as 2.3×10^(15)Ωcm and 324.2 kV mm^(-1),***,it also presents extremely high tensile strength of 193.6 MPa and thermal decomposition temperature of 640°C,showing a broad application prospect in high-end thermal management fields such as electronic devices and electrical equipment.

关键词： Poly(p-phenylene-2,6-benzobisoxazole)nanofiber Boron nitride Thermal conductivity Electrical insulation

Mediated electron transfer process in α-MnO_(2)catalyzed Fenton-like reaction for oxytetracycline degradation

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Chinese Chemical Letters 2024年第8期35卷 367-372页

作者： Yiqian Jiang Zihan Yang Xiuru Bi Nan Yao Peiqing Zhao Xu Meng State Key laboratory for Oxo synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China University of Chinese Academy of Sciences Beijing 100049China

In Fenton-like oxidation,the catalyst directly influences the reaction mechanism for the degradation of pollutants from ***,a α-MnO_(2)catalyst(OAm-1)was synthesized via a self-assembly method with the assistance of a ***-1 possessed a large specific surface area of_(2)21 m2/g,abundant mesoporous structures and a large proportion of Mn(III).Further characterization exhibited that OAm-1 had abundant oxygen vacancies and excellent reducibility and *** adsorption and catalytic ability of OAm-1 were studied in the degradation of oxytetracycline(OTC)via the activation of hydrogen peroxide(H_(2)O_(2)).Through the radical quenching experiments,electron resonance spectroscopy(EPR),X-ray photoelectron spectroscopy(XPS)and Fourier-transform infrared spectroscopy(FT-IR)analysis,Mn(III)of OAm-1 was proved to be the active sites for the chemisorption of *** electrochemical ex-periments and analysis have shown that a process of electron transfer mediated by OAm-1 occurred be-tween the pollutant and H_(2)O_(2)during a Fenton-like *** work experimentally verifies the elec-tron transfer process dominated nonradical mechanism overα-MnO_(2),which is helpful for understanding the catalytic mechanism of the Fenton-like oxidation.

关键词： Mediated electron transfer Hydrogen peroxide Oxidative degradation Manganese oxide Fenton oxidation

Copper-catalyzed enantioselective desymmetrizing C(sp^(2))-H functionalization of azide-ynamides via α-imino copper carbenes

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Science China Chemistry 2024年第9期67卷 2982-2988页

作者： En-He Huang Li-Gao Liu You-Wei Yin Hao-Xuan Dong Ji-Jia Zhou Xin Lu Bo Zhou Long-Wu Ye Key laboratory for Chemical Biology of Fujian Province and State Key laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China State Key laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

α-Imino metal carbenes are versatile intermediates in organic synthesis,and have broad applications in the assembly of divergent ***,the catalytic enantioselective desymmetrization based onα-imino metal carbenes has not been developed to ***,we disclose an enantioselective desymmetrizing C(sp^(2))-H functionalization of azide-ynamides viaα-imino copper carbenes,leading to the efficient assembly of divergent chiral indoloazepines in generally moderate to excellent yields with high ***,this reaction represents the first enantioselective desymmetrization based onα-imino metal *** synthetic transformations and biological tests show the potential utility of this ***,computational studies are employed to elucidate the reaction mechanism and the origin of enantioselectivity.

关键词： enantioselective desymmetrization metal carbenes copper catalysis nitrene transfer alkynes