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A New Spirostanol Saponin from Dioscorea futshauensis

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Chinese Chemical Letters 2001年第7期12卷 613-616页

作者： Hong Wei LIU hisayoshi kobayashi Ge Xia QU Xin Sheng YAO Department of Natural Products Chemistry Shenyang Pharmaceutical UniversityShenyang 110015 Institute of Molecular&Cellular Biosciences The University of TokyoTokyoJapan 113

A new spirostanol saponin presenting strong activity of inducing morphological deformation of Pyricularia oryzae mycelia was isolated from Dioscorea futshauensis R. Kunth by bioactivity-guided fractionation. The structure was established as (25S)-spirost-5-en-3 beta, 27-diol-3-O- [alpha -L-rhamnopyranosyl (1 -->2)-beta -D glucopyranosyl (1 -->3)]-beta -D-glucopyranoside on the basis of chemical evidences and spectral analysis, especially by 2D-NMR techniques.

关键词： New spirostanol glycoside Dioscorea futshauensis Pyricularia oryzae

5′-Hydroxyzearalenol,a new β-resorcylic macrolide from Fusarium sp. 05ABR26

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Chinese Chemical Letters 2008年第9期19卷 1089-1092页

作者： Ling Ling Zhao Yue Gai hisayoshi kobayashi Chang Qi Hu Hui Ping Zhang Department of Natural Products Chemistry School of Pharmacy Fudan University Shanghai 200032 China Institute of Molecular and Cellular Biosciences The University of Tokyo Tokyo 113-0032 Japan

A new β-resorcylic macrolide, 5＇-hydroxyzearalenol （1）, was isolated from the culture broth of a marine-derived fungus Fusarium sp. 05ABR26. Three known compounds, zearalenone （2）, 8＇-hydroxyzearalenone （3） and zearalenol （4） were also isolated. The structure and relative stereochemistry of 1 were elucidated on the basis of spectroscopic data and single-crystal X-ray diffraction data. Compound 2 displayed potent inhibitory activity against Pyricularia oryzae with a MIC value of 6.25 μg/mL, while compound 3 was much less active; however, 1 and 4 showed no obvious activity.

关键词： 5'-Hydroxyzearalenol Fusarium sp. X-ray diffraction data Pyricularia oryzae

Visible Light-Induced Photocatalysis on Carbon Nitride Deposited Titanium Dioxide： Hydrogen Production from Sacrificial Aqueous Solutions

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Chinese Journal of Chemistry 2017年第2期35卷 165-172页

作者： Shinya Higashimoto Kohji Hikita Masashi Azuma Mari Yamamoto Masanari Takahashi Yoshihisa sakata Masaya Matsuoka hisayoshi kobayashi Department of Applied Chemistry College of Engineering Osaka Institute of Technology 5-16-10miya Asahi-ku Osaka 535-8585 Japan Osaka Municipal Technical Research Institute 1-6-50 Morinomiya Joto-ku Osaka 536-8553 Japan Graduate School of Science andEngineering Yamaguchi University 2-16-1 Tokiwadai Ube 755-8611 Japan Department of Applied Chemistry Graduate School of Engineering Osaka Prefecture University 1-1 Gakuen-cho Naka-ku Sakai Osaka 599-8531 Japan Department of Chemistry and Materials Technology Kyoto Institute of Technology Matsugasaki Sakyo-ku Kyoto 606-8585 Japan

Carbon and nitrogen species-involved TiO2 （CN-TiO2） were systematically synthesized by thermal condensa- tion of cyanuric acid on the TiO2 surface. And the photocatalytic reactions for H2 production from sacrificial aque- ous solutions were performed on several CN-TiO2 photocatalyst under visible-light irradiation. The photocatalytic activity of the CN-TiO2 was influenced by total amounts of carbon and nitrogen species, and the preferable activity was ten times higher than that of pristine carbon nitride. Here, the states of the CN-TiO2 photocatalyst were charac- terized by XPS, FT-IR and UV-Vis spectroscopy as well as DFT calculations. The photo-electrochemical measure- ments confirmed that the enhancement of H2 production is associated with effective charge separation under photo- excitation of highly dispersed carbon nitride on the TiO2 surface.

关键词： carbon nitride TiO2 visible light photo-electrochemistry DFT calculation sacrificial H2 production

Green catalytic oxidation of benzyl alcohol over Pt/ZnO in base‐free aqueous medium at room temperature

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Chinese Journal of Catalysis 2018年第6期39卷 1081-1089页

作者： Juanjuan Liu Shihui Zou Jiachao Wu hisayoshi kobayashi Hongting Zhao Jie Fan College of Materials ＆ Environmental Engineering Hangzhou Dianzi University Hangzhou 310036 Zhejiang China Key Lab of Applied Chemistry of Zhejiang Province Department of Chemistry Zhejiang University Hangzhou 310027 Zhejiang China Department of Chemistry and Materials Technology Kyoto Institute of Technology Matsugasaki Sakyo‐ku Kyoto 606‐8585 Japan

The selective oxidation of alcohol using molecular oxygen as an oxidant and water as a green sol‐vent is of great interest in green chemistry. In this work, we present a systematic study of a Pt/ZnO catalyst for the selective oxidation of benzyl alcohol at room temperature under base‐free aqueous conditions. Experimental observations and density functional theory calculations suggest that ZnO as a support can facilitate the adsorption of benzyl alcohol, which subsequently reacts with the activated oxygen species on the Pt catalyst, producing benzaldehyde. The resulting solid achieves a high conversion（94.1 ± 5.1% in 10 h） of benzyl alcohol and nearly 100% selectivity to benzalde‐hyde with ambient air as the oxidant. In addition, by introducing a small amount of Bi（1.78 wt%） into Pt/ZnO, we can further enhance the activity by 350%.

关键词： Pt/ZnO Selective oxidation Benzyl alcoholC–Hactivation Aqueous medium Room temperature

Selective suppression of toluene formation in solvent-free benzyl alcohol oxidation using supported Pd-Ni bimetallic nanoparticles

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Chinese Journal of Catalysis 2017年第11期38卷 1870-1879页

作者： Jianwei Che Mengjia Hao Wuzhong Yi hisayoshi kobayashi Yuheng Zhou Liping Xiao Jie Fan Key Lab of Applied Chemistry of Zhejiang Province Department of Chemistry Zhejiang University Hangzhou 310027 Zhejiang China Department of Chemistry and Materials Technology Kyoto Institute of Technology Kyoto 606‐8585 Kyoto Prefecture Japan

The solvent‐free oxidation of benzyl alcohol was studied using supported Pd‐Ni bimetallic *** with monometallic Pd,the addition of Ni to Pd was found to be effective in suppressing the nondesired product toluene,thereby enhancing the selectivity towards *** result was attributed to a dual effect of Ni addition:the weakening of dissociative adsorption of benzyl alcohol and the promotion of oxygen species involved in the oxidation pathway.

关键词： Palladium‐nickel Bimetallic nanoparticle Benzyl alcohol Toluene Solvent‐free Oxidation

表面Lewis酸碱反应对ZnO可见光产氢性能的影响

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表面Lewis酸碱反应对ZnO可见光产氢性能的影响

Surface coupling of methyl radicals for efficient low‐temperature oxidative coupling of methane

中国化学会第29届学术年会

作者：邹世辉刘娟娟 hisayoshi kobayashi 范杰浙江大学化学系日本京都工艺纤维大学

氧化锌（ZnO）是一种重要的宽带隙半导体,在压电器件,光发射器件,光催化等方面有很广泛的应用。但是,ZnO在作为光催化剂时,由于只能吸收紫外光,易光腐蚀,而且光生电子和空穴易复合,其应用受到了很大的限制,也一直被认为是一种低效的光... 详细信息

氧化锌（ZnO）是一种重要的宽带隙半导体,在压电器件,光发射器件,光催化等方面有很广泛的应用。但是,ZnO在作为光催化剂时,由于只能吸收紫外光,易光腐蚀,而且光生电子和空穴易复合,其应用受到了很大的限制,也一直被认为是一种低效的光分解水催化剂。1本文通过在ZnO/HCHO水溶液中直接加入Bi（NO3）3的方法,使得它们在可见光下表现出较好的产氢活性及光稳定性。通过XRD,XPS,UV-Vis,SEM,HRTEM及DFT理论计算,我们发现ZnO/Bi（NO3）3体系的可见光活性主要来源于表面Bi（NO3）3与ZnO的Lewis酸碱反应。这一反应不仅仅改变了ZnO的表面结构（价态,形貌等）,而且也改变了ZnO的表面能带结构,从而使得ZnO具有较好的可见光催化产氢性能及光稳定性。

关键词：可见光产氢氧化锌 Lewis酸碱反应

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Chinese Journal of Catalysis 2021年第7期42卷 1117-1125页

作者： Shihui Zou Zhinian Li Qiuyue Zhou Yang Pan Wentao Yuan Lei He Shenliang Wang Wu Wen Juanjuan Liu Yong Wang Yonghua Du Jiuzhong Yang Liping Xiao hisayoshi kobayashi Jie Fan Key Laboratory of Applied Chemistry of Zhejiang Province Department of ChemistryZhejiang UniversityHangzhou 310036ZhejiangChina National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029AnhuiChina School of Materials Science and Engineering Zhejiang UniversityHangzhou 310027ZhejiangChina College of Materials&Environmental Engineering Hangzhou Dianzi UniversityHangzhou 310036ZhejiangChina National Synchrotron Light Source II Brookhaven National Laboratory Upton NY11973USA Emertus Professor of Kyoto Institute of Technology MatsugasakiSakyo‐kuKyoto 606‐8585Japan

Selective coupling of methyl radicals to produce C_(2) species(C2H4 and C2H6)is a key challenge for oxidative coupling of methane(OCM).In traditional OCM reaction systems,homogeneous transformation of methyl radicals in O_(2)‐containing gases are uncontrollable,resulting in limited C_(2) selectivity and ***,we demonstrate that methyl radicals generated by La_(2)O_(3)at low reaction temperature can selectively couple on the surface of 5 wt%Na2WO4/SiO_(2).The controllable surface coupling against overoxidation barely changes the activity of La_(2)O_(3)but boosts the C_(2)selectivity by three times and achieves a C_(2)yield as high as 10.9%at bed temperature of only 570℃.Structure‐property studies suggest that Na_(2)WO_(4) nanoclusters are the active sites for methyl radical *** strong CH_(3)·affinity of these sites can even endow some methane combustion catalysts with OCM *** findings of the surface coupling of methyl radicals open a new direction to develop OCM *** bifunctional OCM catalyst system,which composes of a methane activation center and a CH_(3)·coupling center,may deliver promising OCM performance at reaction temperatures below the ignition temperature of C2H6 and C2H4(~600℃)and is therefore more controllable,safer,and certainly more attractive as an actual process.

关键词： Oxidative coupling of methane Bifunctional catalysis Methyl radicals Surface coupling La_(2)O_(3) Na_(2)WO_(4)/SiO_(2)

AuCN纳米颗粒的自由基诱导一步法绿色合成路线

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AuCN纳米颗粒的自由基诱导一步法绿色合成路线

Tuning catalytic selectivity of propane oxidative dehydrogenation via surface polymeric phosphate modification on nickel oxide nanoparticles

中国化学会第28届学术年会

作者：李仁宏闫晓庆邹世辉汤禹 hisayoshi kobayashi 范杰浙江大学京都纤维工艺大学

＜正＞黄金（Au）在化学（尤其是现代催化化学）研究史上占有极其重要的地位。一般而言,Au是惰性的贵金属材料,但Au其实具备丰富的配位和金属有机化学。传统的冶金方法是利用氰化物将Au从低品位的矿中

关键词：自由基 AuCN 绿色一步法纳米颗粒

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Chinese Journal of Catalysis 2019年第7期40卷 1057-1062页

作者： Kaimin Du Mengjia Hao Zhinian Li Wei Hong Juanjuan Liu Liping Xiao Shihui Zou Jie Fan Key Lab of Applied Chemistry of Zhejiang Province Department of ChemistryZhejiang UniversityHangzhou 310027ZhejiangChina College of Materials & Environmental Engineering Hangzhou Dianzi UniversityHangzhou 310018ZhejiangChina Department of Chemistry and Materials Technology Kyoto Institute of TechnologyMatsugasakiSakyo-kuKyoto 606-8585Japan

Thermal stability has long been recognized as a major limitation for the application of ligand modification in high-temperature reactions. Herein, we demonstrate polymeric phosphate as an efficient and stable ligand to tune the selectivity of propane oxidative dehydrogenation. Beneficial from the weakened affinity of propene, NiO modified with polymeric phosphate shows a selectivity 2–3 times higher than NiO towards the production of propene. The success of this regulation verifies the feasibility of ligand modification in high-temperature gas-phase reactions and shines a light on its applications in other important industrial reactions.

关键词： Nickel oxide nanoparticle Surface polymeric phosphate Propane oxidative dehydrogenation Tuning selectivity Adsorption