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Catalytic asymmetric(3+3)cycloaddition between different 2-indolylmethanols

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Science China chemistry 2024年第8期67卷 2629-2636页

作者： Tianzhen Li Sijia Liu Shufang Wu Qi Cheng Qun Chen Yinchun Jiao Yuchen Zhang Feng Shi school of Petrochemical Engineering School of Materials ScienceEngineeringChangzhou UniversityChangzhou 213164China Research Center of Chiral Functional Heterocycles School of Chemistry and Materials ScienceJiangsu Normal UniversityXuzhou 221116China school of chemistry and Chemical Engineering Hunan University of Science and TechnologyXiangtan 411201China school of chemistry and Chemical Engineering Henan Normal UniversityXinxiang 453007China

The catalytic asymmetric(3+3)cycloaddition between different 2-indolylmethanols has been established,in which a series of chiral indole-fused six-membered heterocycles were constructed in high yields with excellent *** work not only has established the first catalytic asymmetric cycloaddition between different 2-indolylmethanols but also provided a powerful strategy for constructing enantioenriched indole-fused six-membered ***,biological evaluation discovered some products with promising antitumor ***,theoretical calculations performed on the reaction pathway and activation mode provide an in-depth understanding of this catalytic asymmetric(3+3)cycloaddition among different 2-indolylmethanols,which will advance the understanding of the chemistry of indolylmethanols.

关键词： asymmetric organocatalysis chiral phosphoric acid cycloaddition enantioselectivity 2-indolylmethanol

Graphdiyne(C_(n)H_(2n-2))as an"electron transfer bridge"boosting photocatalytic hydrogen evolution over Zn_(0.5)Co_(0.5)S/MoS_(2)S-scheme heterojunction

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Rare Metals 2024年第5期43卷 1999-2014页

作者： Mei Li Jing-Zhi Wang Zhi-Liang Jin school of chemistry and Chemical Engineering North Minzu UniversityYinchuan 750021China school of chemistry and Chemical Engineering Ningxia Key Laboratory of Solar Chemical Conversion TechnologyKey Laboratory for Chemical Engineering and TechnologyState Ethnic Affairs CommissionNorth Minzu UniversityYinchuan 750021China

In the process of photocatalytic water cracking,the migration rate and utilization rate of photogenerated charges determine the hydrogen evolution performance of the *** this paper,a carbon isotope superconducting material graphdiyne(GDY)is prepared by mechanical ball milling and introduced into the S-scheme heterojunction Zn_(0.5)Co_(0.5)S/MoS_(2)inorganic *** terms of hydrogen evolution kinetics,GDY acts as an electron bridge,not only accelerating the migration of photogenerated carriers but also improving the utilization of photogenerated ***,the large twodimensional layer provides more loading and anchoring points for Zn_(0.5)Co_(0.5)S/MoS_(2),which increases the number of active *** ternary composite catalyst 20%GDY/Zn_(0.5)Co_(0.5)S/MoS_(2)(20-GCSM)generates 69.94μmol of hydrogen(5 h)in triethanolamine *** is 2.97 and1.80 times higher than Zn_(0.5)Co_(0.5)S and Zn_(0.5)Co_(0.5)S/MoS_(2),*** the cyclic experiment,it still has stable hydrogen evolution performance after standing for24 h(under dark conditions).In addition,the potential mechanism of photocatalytic hydrogen evolution is demonstrated through in-situ X-ray photoelectron *** work provides a reference for further research in the field of introducing carbon materials into photocatalytic systems and improving the utilization of photogenerated charges.

关键词： Graphdiyne S-scheme heterojunction Electron transfer bridge Hydrogen production

Porous Ti_(3)C_(2)T_(x) MXene nanosheets sandwiched between polyimide fiber mats for electromagnetic interference shielding

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Nano Research 2024年第3期17卷 2070-2078页

作者： Wenhao Liang Juntao Wu Shan Zhang Pei-Yan Zhao Yi Cong Yongqiang Guo Guang-Sheng Wang Key Laboratory of Bioinspired Smart Interfacial Science and technology of Ministry of Education School of ChemistryBeihang UniversityBeijing 100191China

With the rapid development of wireless communication technology and electronic devices,the issue of electromagnetic interference(EMI)is becoming increasingly *** a new and flexible electromagnetic interference shielding material has become a challenging ***,a sandwich-structured EMI shielding composite film was prepared using electrospinning and vacuum filtration *** this process,a porous MXene was synthesized through a reaction with cobalt acetate and served as the intermediate layer in the composite film to shield electromagnetic *** electrospun polyimide(PI)fibers were used as the top and bottom layers of the composite film,which can protect the porous MXene from *** lightweight and flexible composite film integrates electromagnetic interference shielding and thermal insulation capabilities,showing excellent comprehensive *** composite film achieves an EMI shielding effectiveness of 48.8 dB in X-band(8.2–12.4 GHz),and absolute shielding effectiveness of the composite film reached a satisfying 4142.43(dB·cm^(2))/*** to the design of a multi-layer porous structure,the density of the composite film is 0.65 g/***,the thermal conductivity of the film is 0.042 W/(m·K)due to the clamping of electrospun PI fibers,showing excellent thermal insulation ***,the composite film exhibits excellent high and low-temperature *** summary,this work provides a feasible strategy for preparing a lightweight polymer-based EMI shielding film.

关键词： porous MXene polyimide electromagnetic interference shielding thermal insulation

Atomic-level coupled RuO_(2)/BaRuO_(3) heterostructure for efficient alkaline hydrogen evolution reaction

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Journal of Energy chemistry 2024年第1期88卷 356-362,I0009页

作者： Yueying Yan Tian Meng Yuting Chen Yang Yang Dewen Wang Zhicai Xing Xiurong Yang State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina school of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina

The slow water dissociation is the rate-determining step that slows down the reaction rate in alkaline hydrogen evolution reaction(HER).Optimizing the surface electronic structure of the catalyst to lower the energy barrier of water dissociation and regulating the binding strength of adsorption intermediates are crucial strategy for boosting the catalytic performance of *** this study,RuO_(2)/BaRuO_(3)(RBRO)heterostructures with abundant oxygen vacancies and lattice distortion were in-situ constructed under a low temperature via the thermal decomposition of *** RBRO heterostructures obtained at 550℃ exhibited the highest HER activity in 1 M KOH,showing an ultra-low overpotential of 16 mV at 10 mA cm^(-2)and a Tafel slope of 33.37 m V dec^(-1).Additionally,the material demonstrated remarkable durability,with only 25 mV of degradation in overpotential after 200 h of stability testing at 10 mA cm^(-2).Density functional theory calculations revealed that the redistribution of charges at the heterojunction interface can optimize the binding energies of H*and OH*and effectively lower the energy barrier of water *** research offers novel perspectives on surpassing the water dissociation threshold of alkaline HER catalysts by means of a systematic design of heterogeneous interfaces.

关键词： Heterostructure Hydrogen evolution reaction Interfacial electron transfer Oxygen vacancies

A-site assisted perovskite crystallization via ion-exchange MOFs for high efficient and stable perovskite solar cells

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Journal of Energy chemistry 2024年第6期93卷 436-442,I0011页

作者： Xingrui Zhang Jian Zhang Wei Wang Boyuan Hu Yayu Dong Debin Xia Kaifeng Lin Yulin Yang MIIT Key Laboratory of Critical Materials technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina

Here,a novel strategy is proposed targeting the volatility of A-site cations and the disordered arrangement of perovskite grains through employing Cs~+contained metal-organic frameworks In-aip(Cs)obtained by ion-exchange and crystalline *** forces between Cs-O atoms split the pore channels of the pristine In-aip,endowing In-aip(Cs)with multidimensional charge transport channels,In addition,the partially freed Cs~+in the interlayer compensates for the vacancy of A-site cations during the perovskite preparation *** In-aip(Cs)modified perovskite films have a flat morphology,large grains and excellent optoelectronic *** from the high-quality perovskite films and faster charge extraction,the In-aip(Cs)-modified PSCs achieved a champion PCE of 23.03%,superior to the In-aip-modified(22.29%)and control device(21.13%),More importantly,the unencapsulated PSCs modified with In-aip(Cs)exhibited outstanding humidity and thermal *** a period of almost 1000 h,the unencapsulated In-aip(Cs)-modified device retained 85%of its initial PCE after storing in a glove box at 85℃,and retained 87%of the primary PCE upon storage in ambient condition at 25℃under a humidity of 40%.

关键词： Metal-organic frameworks PSCs Stability Defect passivation

Radiation construction and excellent performances of Ag NPs/TiO_(2)/PEG/PVP multifunctional aerogel:Adsorption-photocatalytic degradation,photosensitive antibacterial and cytotoxicity

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Journal of Materiomics 2024年第3期10卷 585-593页

作者： Jin-Yu Yang Dong-Liang Liu Yue-Sheng Li Xiao-Jie Yang Yi Liu school of Nuclear technology and chemistry&Biology/Hubei Key Laboratory of Radiation chemistry and Functional Materials Hubei University of Science and TechnologyXianning437100HubeiChina Key Laboratory of Coal Conversion and New Carbon Materials of Hubei Province School of Chemistry and Chemical EngineeringWuhan University of Science and TechnologyWuhan437100HubeiChina College of chemistry and Chemical Engineering Tiangong UniversityTianjin300387China

A cutting-edge method known as photocatalytic antibacterial technology can effectively eliminate drug-resistant bacterial strains and boast a wide-ranging antimicrobial *** the study,a novel Ag NPs/TiO_(2)/PEG/PVP(ATPP)aerogel photocatalyst was synthesized by an electron beam in-situ radiation method using polyethylene glycol(PEG),polyvinylpyrrolidone(PVP),AgNO_(3),and TiO_(2)as raw *** was characterized by X-ray diffraction spectroscopy(XRD),X-ray photoelectron spectroscopy(XPS)and solid ultraviolet diffuse reflectance spectroscopy(UV-Vis DRS).The results demonstrated that silver ions were reduced to silver nanoparticles by electron beam radiation *** the same time,the doping of silver nanoparticles(Ag NPs)enhanced visible-light *** degradation rate of methylene blue(MB)on 5%(in mass)ATPP could reach 81%under visible light for 180 *** coli(***)and Staphylococcus aureus(***)were used as model bacteria to explore the antimi-crobial properties of ATPP by zone of the inhibition method,plate counting method and live/dead bacterial *** antibacterial experiments showed that the antibacterial effect of ATPP was ***,MTT assay and Hoechst33342/PI double staining were used to prove that the composite had good *** aerogel photocatalytic material has the potential to decrease microbial presence in both medical and environmental settings,making it a valuable tool for such applications.

关键词： Ag NPs/TiO_(2)/PEG/PVP aerogel Electron beam radiation Adsorption-photocatalytic Photosensitive antibacterial Cytotoxicity

Self-optimized H-adsorption affinity of CuRu alloy cocatalysts towards efficient photocatalytic H_(2)evolution

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Journal of Materials Science & technology 2024年第7期174卷 168-175页

作者： Meiya Wang Ping Wang Xuefei Wang Feng Chen Huogen Yu school of chemistry Chemical Engineering and Life Sciencesand School of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070China Laboratory of Solar Fuel Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430078China

In addition to the electron transfer,the appropriate H-adsorption affinity of active centers on the metal cocatalyst surface is quite important for high hydrogen-production activity of cocatalyst-modified *** typical Cu and Ru metal cocatalysts clearly exhibit a weak Cu-H bond and a strong Ru-H bond,respectively,resulting in limited activity for photocatalytic H_(2)*** this work,an ingenious strategy of self-optimized H-adsorption affinity in CuRu alloy cocatalyst is developed to simultaneously reinforce the Cu-H bond and weaken the Ru-H bond by the intrinsic electron transfer from Cu to Ru *** CuRu alloy nanoparticles(2-3 nm)were deposited on the TiO_(2)surface to prepare CuRu/TiO_(2)through a one-step photoreduction *** tests exhibited that the highest H_(2)-production rate of CuRu/TiO_(2)photocatalyst reached up to 5.316 mmol h^(-1)g^(-1),which was 24.80,1.86,and 2.60 times higher than that of the TiO_(2),Cu/TiO_(2),and Ru/TiO_(2),*** on the characterization results and theoretical calculations,the CuRu alloy cocatalyst exhibits excellent self-optimized H-adsorption affinity via the spontaneous electron transfer from Cu to Ru atom,which can greatly accelerate the photocatalytic H_(2)-production rate of TiO_(2).This work provides a feasible idea for the self-optimized H-adsorption affinity of metal active sites in the photocatalytic H_(2)-generation field.

关键词： TiO_(2) CuRu alloy Cocatalyst Self-optimized H-adsorption affinity Photocatalytic H_(2)generation

General radical difluoromethylation using difluoroacetic anhydride via photoredox catalysis

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Science China chemistry 2024年第8期67卷 2637-2646页

作者： Meng He Yankai Yang Heng Zhang Zhipeng Guan Zhi-Bing Dong Hong Yi Aiwen Lei school of chemistry and Environmental Engineering Wuhan Institute of TechnologyWuhan 430205China College of chemistry and Molecular Sciences and Institute for Advanced Studies(IAS) Wuhan UniversityWuhan 430072China

CF_(2)H-containing molecules play pivotal roles in diverse fields from medicinal chemistry to materials science. However, the application of existing CF_(2)H reagents as a source of CF_(2)H radical is limited by their reactivity and preparation. Herein, we develop a simple and general visible-light-catalyzed radical difluoromethylation reaction of alkenes, dienes, and heteroaromatics using commercially available, easy-to-handle, and low-cost difluoroacetic anhydride as the CF_(2)H reagent. This scalable protocol enables the convenient synthesis of a range of CF_(2)H-containing compounds under mild conditions, exhibiting a broad substrate scope and functional group tolerance. Potential applications are further demonstrated by gram-scale synthesis, sunlight experiments, derivatization experiments as well as the synthesis of bioactive molecules.

关键词： radical difluoromethylation alkenes/dienes/heteroaromatics difluoroacetic anhydride photoredox

Accelerating solar driven CO_(2) reduction via sulfur-doping boosted water dissociation and proton transfer

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Nano Research 2024年第3期17卷 1056-1065页

作者： Ke Yan Liang Chen Yangguang Hu Ting Wang Cong Chen Chao Gao Youju Huang Benxia Li school of chemistry and Chemical Engineering Key Laboratory of Surface&Interface Science of Polymer Materials of Zhejiang ProvinceZhejiang Sci-Tech UniversityHangzhou 310018China College of Material Chemistry and Chemical EngineeringKey Laboratory of Organosilicon Chemistry and Material TechnologyMinistry of EducationHangzhou Normal UniversityHangzhou 311121China school of chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China

Exploring efficient photocatalysts for solar driven CO_(2) reduction with water(H_(2)O)as a proton donor is highly imperative but remains a great challenge because the synchronous enhancement of CO_(2) activation,H_(2)O dissociation and proton transfer is hardly achieved on a ***,the sluggish H_(2)O dissociation impedes the photocatalytic CO_(2) reduction reaction involving multiple proton–electron coupling transfer ***,a sulfur-doped BiOCl(S-BiOCl)photocatalyst with abundant oxygen vacancies(OV)is developed,which exhibits broadband-light harvesting across solar spectrum and distinct photothermal effect due to *** photocatalytic CO_(2) reduction with H_(2)O in a gas–solid system,the high CO yield of 49.76μmol·g_(cat)^(-1)·h^(-1) with 100%selectivity is achieved over the S-BiOCl catalyst under a simulated *** H_(2)O-assisted CO_(2) reduction reaction on S-BiOCl catalyst is triggered by photocatalysis and the photothermal heating further enhances the reaction *** kinetic isotope experiments indicate that the sluggish H_(2)O dissociation affects the whole photocatalytic CO_(2) reduction *** presence of oxygen vacancies promotes the adsorption and activation of H_(2)O and CO_(2),and the doped S sites play a crucial role in boosting H_(2)O dissociation and accelerating the dynamic migration of hydrogen *** a result,the ingenious integration of OV defects,S sites and photothermal effect in S-BiOCl catalyst conjointly contributes to the significant improvement in photocatalytic CO_(2) reduction performance.

关键词： BiOCl sulfur doping photocatalytic CO_(2)reduction H_(2)O activation proton feeding