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Chinese Chemical Letters 2024年第2期35卷 415-419页

作者： Yufen Lv Hongyu Ding Jinmao You Wei Wei Dong Yi Key Laboratory of Catalytic Conversion and Clean Energy in Universities of Shandong Province School of Chemistry and Chemical EngineeringQufu Normal UniversityQufu 273165China College of Chemistry and Chemical Engineering Shaoxing UniversityShaoxing 312000China School of Pharmacy Southwest Medical UniversityLuzhou 646000China

An additive-free and environmentally friendly strategy has been realized for the construction of S-substituted isothioureas through visible-light-induced multicomponent reaction starting fromα-diazoesters,aryl isothiocyanates,amines and cyclic ethers.This methodology features simple operation,mild reaction conditions,favorable functional group tolerance,easily available starting materials and high efficiency.

关键词： visible-light Additive-free Four-component reaction S-Substituted isothioureas

A unique and well-designed 2D graphitic carbon nitride with sponge-like architecture for enhanced visible-light photocatalytic activity

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Journal of Materials Science & Technology 2023年第28期159卷 99-111页

作者： Mahdieh Razi Asrami Milad Jourshabani Min Hee Park Daiha Shin Byeong-Kyu Lee Department of Civil and Environment Engineering University of UlsanDaehakro 93NamguUlsan 680-749Republic of Korea Western Seoul Center Korea Basic Science InstituteSeoul 03759Republic of Korea

A unique and well-designed 2D graphitic carbon nitride(g-CN)with sponge-like architecture has been successfully synthesized by engineering supramolecular self-assembly and well-organized SiO 2 nanoparti-cles.The resulting material showed great optical and textural characteristics with plenty of open and uni-form pores,which are very helpful whether for multiple light scattering or mass transfer.The formation of boosted delocalizedπ-conjugated electrons at the molecular level and condensed heptazine building blocks result in enhanced carrier density and charge transfer dynamics.Optical emission spectroscopy and time-resolved fluorescence lifetime(TRPL)strongly confirmed the enhancement of light harvesting and prolonged charge carrier lifetime.The optimized sample exhibited a degradation performance of 95%of bisphenol A(BPA,10 mg L-1)after 60 min under visible-light irradiation at pH=5.All the scavenging experiments,probing experiments as well as electron paramagnetic resonance(EPR)confirm that•O 2-is the dominant reactive species that fragments bisphenol A.Interestingly,density functional theory(DFT)calculations unveil that the BPA interaction with a modified g-CN containing porous structure is energeti-cally more favorable than non-porous pure g-CN.Moreover,the toxicity assessment showed that the final degradation products were placed in the non-harmful category based on acute and chronic toxicity.This study presents a promising strategy to modify the g-CN properties and provides an efficient technique for boosting its visible-light photocatalytic activity.

关键词： Sponge-like Carbon nitride Photocatalysis visible-light

Synergistic interaction of three-dimensional ZnCdS@MoS2 heterostructures for high-efficiency visible-light photocatalytic degradation of dyes

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Progress in Natural Science:Materials International 2023年第4期33卷 442-449页

作者： Yingjiao Zhai Haowen He Mingze Xu Hongbin Zhao Jinhua Li Ministry of Education Key Laboratory for Cross-Scale Micro and Nano Manufacturing Nanophotonics and Biophotonics Key Laboratory of Jilin Province State Key Laboratory of High Power Semiconductor Lasers Changchun University of Science and Technology State Key Laboratory of Advanced Materials for Smart Sensing General Research Institute for Nonferrous Metals

High-performance photocatalysts should urgently be developed to efficiently solve serious environmental problems. Herein, we successfully synthesized a novel, visible-light activated, three-dimensional ZnCdS@MoS2photocatalyst using a simple, two-step hydrothermal process. Based on reaction time-dependence, the growth mechanism of “oriented attachment” of the ZnCdS@MoS2heterostructure is described in detail. The photodegradation of methylene blue(MB) indicated that the prepared sample has an outstanding photocatalytic activity owing to the accelerated photogenerated electron production rate, inhibited electron–hole pair recombination,improved visible light–utilization rate, and increased specific surface area. According to our experimental results,the degradation rate of MB using the ZnCdS@MoS2nanocomposite was as high as 99.3% after 100 min of visible-light irradiation. The photocatalyst remained stable without any obvious decrease in activity even after three cycles of use. This study provides a strong support for the design of high-performance photocatalysts and their application in optoelectronic devices.

关键词： Dye Heterostructure Photocatalytic visible-light ZnCdS@MoS2

Photocatalyst-free visible-light-mediated three-component reaction ofα-diazoesters, cyclic ethers and NaSCN to access organic thiocyanates

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Chinese Chemical Letters 2023年第2期34卷 198-201页

作者： Zhiwei Wang Na Meng Yufen Lv Wei Wei Huilan Yue Guofu Zhong School of Chemistry and Chemical Engineering Qufu Normal UniversityQufu 273165China Qinghai Provincial Key Laboratory of Tibetan Medicine Research and CAS Key Laboratory of Tibetan Medicine Research Northwest Institute of Plateau BiologyXining 810008China

A facile and environmentally friendly visible-light-induced three-component reaction of α-diazoesters,cyclic ethers and Na SCN to construct organic thiocyanates has been developed at room temperature. This reaction could occur under photocatalyst-and additive-free conditions to afford a number of organic thiocyanates with moderate to good yield and favorable functional group tolerance.

关键词： Photocatalyst-free visible-light Three-component reaction Organic thiocyanates

Recyclable Cu/g-C_(3)N_(4)nanometric semiconductor catalyzed N-formylation of amines via photocatalytic aerobic oxidative C-C bond cleavage of aldehydes under visible-light irradiation

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Chinese Chemical Letters 2023年第6期34卷 354-357页

作者： Zeyao Liang Jiabao Guo Peng Wang Li Zhu Xiaoquan Yao Department of Applied Chemistry School of Material Science and TechnologyNanjing University of Aeronautics and AstronauticsNanjing 210016China Department of Chemistry School of PharmacyNanjing Medical UniversityNanjing 211166China

Due to its difficulty and complexity,the cleavage and subsequent functionalization of the C(sp^(3))-C(sp^(3))single bond has received less attention than the C-C bond formation reactions that have been extensively studied.Herein,by utilizing Cu/g-C_(3)N_(4)nanometric semiconductor as a recyclable photocatalyst,an aerobic oxidative C-C bond cleavage of aldehydes was developed with the promotion of amines under visible light irradiation.Based on the reaction,phenylacetaldehyde was selected as a highly efficient formylation reagent for amines.Under blue light irradiation,good to excellent yields of formamides were achieved for various amines in 1 atm oxygen atmosphere at room temperature.This methodology offers a practical,neutral and gentle alternative to the preparation of formamides.

关键词： Photocatalytic C-C bond cleavage N-Formylation of amines Cu/g-C_(3)N_(4) Nanometric semiconductor visible-light

visible-light-initiated 4CzIPN catalyzed multi-component tandem reactions to assemble sulfonated quinoxalin-2(1H)-ones

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Chinese Chemical Letters 2022年第3期33卷 1479-1482页

作者： Zhiwei Wang Qishun Liu Ruisheng Liu Zhongyin Ji Yan Li Xiaohui Zhao Wei Wei School of Chemistry and Chemical Engineering Qufu Normal UniversityQufu 273165China Qinghai Provincial Key Laboratory of Tibetan Medicine Research and Key Laboratory of Tibetan Medicine Research Northwest Institute of Plateau BiologyChinese Academy of SciencesQinghai 810008China

A mild and efficient photochemical multi-component tandem reaction of quinoxalin-2(1H)-ones, alkenes and sulfinic acids is reported. This tandem reaction could be conveniently carried out at room temperature by employing 4Cz IPN as the metal-free photocatalyst and dioxygen(air) as the environmentally benign oxidant. A number of sulfonated quinoxalin-2(1H)-ones were obtained in satisfactory yields with favorable functional group tolerance. Radical trapping experiment and fluorescence quenching experiments were performed to elucidate this visible-light mediated radical reaction process.

关键词： visible-light Multi-component reaction Radical process Sulfonated quinoxalin-2(1H)-ones

Interstitial nitrogen-induced efficiency alcohol oxidation over heterogeneous N–CoMn_(2)O_(4) catalyst under visible-light

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Green Synthesis and Catalysis

Green Synthesis and Catalysis 2023年第4期4卷 293-299页

作者： Hongwei Li Yurong Zhang Jun Tang Guozheng Huang Ping Cui Qingping Ke College of Chemistry and Chemical Engineering Anhui University of TechnologyMaanshan 243002China

Developing highly efficient and recyclable photocatalysts through harvesting solar light as energy is crucial to oxidation for industrial implementation,especially for simple transition metal oxidic catalysts without precious/heavy/rare metal dopants.Herein,we like to report the use of nitrogen-doped CoMn_(2)O_(4) oxide(N–CoMn_(2)O_(4))as a heterogeneous catalyst for efficient oxidation of various alcohols such as p/m/o-methyl-substituted aromatic alcohols,p-substituted aromatic alcohols including electron-donating and electron-withdrawing substituents,heterocycle-based alcohols and secondary aromatic alcohols to the corresponding aldehydes/ketones,under visible light(>420 nm)illumination and mild condition of oxygen as oxidant and room temperature.The relation of various Co-based oxides to their catalytic performance was studied.It is shown that the Co^(2+)species in N–CoMn_(2)O_(4),obviously increased by the doping of nitrogen,are acted as catalytic active species coupled with the synergistic effect between Co and Mn species for the enhanced visible-light selective oxidation of alcohols to aldehydes.A plausible catalytic mechanism is proposed basis of control experiments and published studies,which suggests that this oxidation process probably occurs on Co^(2+)þsites via an ionic reactive oxygen species pathway and ^(1)O2 and O2⋅^(-)species are the reactive oxygen species.This simple transition metal oxide-catalyzed aerobic oxidation provides a green alternative for the manufacture of aldehydes/ketones from alcohols.

关键词： Interstitial nitrogen Alcohol oxidation Room temperature CoMn_(2)O_(4) visible-light

Enzyme-like C-H Oxidation of Glucosides Promoted by visible light

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CCS Chemistry 2022年第11期4卷 3599-3608页

作者： Mingzhong Wu Qian Jiang Qiong Tian Tianyun Guo Feng Cai Shouchu Tang Jian Liu Xiaolei Wang State Key Laboratory of Applied Organic Chemistry Department of Chemistry and School of PharmacyLanzhou UniversityLanzhou 730000 State Key Laboratory of Veterinary Etiological Biology OIE/National Foot and Mouth Disease Reference LaboratoryLanzhou UniversityLanzhou 730000 The National Glycoengineering Research Center Shandong Provincial Key Laboratory of Carbohydrate Chemistry and GlycobiologyShandong UniversityQingdao 266237

To match nature’s prowess at using enzymes to make desired motifs in a regioselective fashion,we explore the use of visible light for the selective oxidation of the hydroxyl group to afford the corresponding ketosaccharide.This highly admirable approach offers several advantages over the enzymatic approach in terms of yields and the scope of substrates.Herein,we report the development of a simple visiblelight-promoted selective oxidation of unprotected glucosides that allows for inexpensive access to valuable keto-saccharide building blocks.The method is employed on a variety of different natural and artificial glucosides,is operationally simple and scalable,and can be used to access keto-saccharides rapidly and inexpensively.

关键词： keto-saccharide selective oxidation unprotected glucoside visible-light

Biogenic C-doped titania templated by cyanobacteria for visible-light photocatalytic degradation of Rhodamine B

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Journal of Environmental Sciences 2014年第5期26卷 1195-1202页

作者： Jiao He Guoli Zi Zhiying Yan Yongli Li Jiao Xie Deliang Duan Yongjuan Chen Jiaqiang Wang The Universities' Center for Photocatalytic Treatment of Pollutants in Yunnan Province Key Laboratory of Medicinal Chemistry for Natural Resources Ministry of Education School of Chemical Sciences & Technology Yunnan University

Cyanobacteria, which occurred in eutrophic water harvest solar light to carry out photosynthesis with high efficiency. In this work, cyanobacteria （Microcystis sp.） were used as biotemplate to synthesize titania structure. The synthesized titania sample had similar morphology to that of the original template in spite of the fragile unicellular structures and extremely high water content of cyanobacterial cells. Incorporation of biogenic C, as well as the morphology inherited from biotemplate improved visible- light absorbance of the titania structure. The sample exhibited higher visible-light photocatalytic activity than commercial titania photocatalyst Degussa P25 for Rhodamine B （RhB） degradation. Compared with those C-doped titania photocatalysts prepared by other methods, cyanobacteria templated titania photocatalyst offer some potential for competitive advantages. The reported strategy opened up a new use for the cyanobacteria. It could also be used for titania in applications such as treatment of polluted water, dye-sensitized solar cells, or other regions.

关键词： cyanobacteria titania C-doped visible-light photocatalysis

Synthesis and enhanced visible-light responsive of C,N,S-tridoped TiO_2 hollow spheres

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Journal of Environmental Sciences 2013年第10期25卷 2150-2156页

作者： Xiaoxia Lin Degang Fu Lingyun Hao Zhen Ding School of Material Engineering Jinling Institute of Technology State Key Laboratory of Bioelectronics Southeast University Jiangsu Centers for Disease Control and Prevention

C,N,S-tridoped TiO2 hollow spheres （labeled as C,N,S-THs） were synthesized using carbon spheres as template and C,N,S-tridoped TiO2 nanoparticles as building blocks. The structure and physicochemical properties of the catalysts were characterized by X- ray diffraction （XRD）, scanning electron microscopy （SEM）, UV-Vis diffuse reflectance spectrum （DRS）, N2 adsorption-desorption isotherms, X-ray photoelectron spectroscopy （XPS） and Photoluminescence emission spectroscopy （PL）. The results showed that the hollow spheres had average diameter of about 200 nm and the shell thickness was about 20 nm. The tridoped TiO2 hollow spheres exhibited strong absorption in the visible-light region. C,N,S-tridoped could narrow the band gap of the THs by mixing the orbit O 2p with C 2p, N 2p and S 3p orbits and shift its optical response from ultraviolet （UV） to the visible-light region. PL analysis indicated that the electron-hole recombination rate of TiO2 hollow spheres had been effectively inhibited when doped with C, N and S elements. The photocatalytic activities of the samples were evaluated for the degradation of X-3B （Reactive Brilliant Red dye, C.I. Reactive Red 2） aqueous solution under visible-light （λ 〉 420 nm） irradiation. It was found that the C,N,S-tridoped TiO2 hollow spheres indicated higher photocatalytic activity than commercial P25 and the undoped counterpart photocatalyst.

关键词： titania C,N,S-tridoped hollow spheres visible-light photocatalysis