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纳米钯催化苄基氯代物与烯丙基硼酸频哪醇酯的羧化Suzuki偶联反应（英文）

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Chinese Journal of Catalysis 2018年第7期39卷 1258-1262页

作者：孙健王加升冯秀娟 yoshinori yamamoto Abdulrahman I.Almansour Natarajan Arumugam Raju Suresh Kumar 包明大连理工大学精细化工国家重点实验室辽宁大连116023 大连理工大学石油与化学工程学院辽宁盘锦124221 东北大学理学研究科化学系日本仙台980-8578 立命馆大学科学技术研究所日本草津志贺525-8577 沙特阿拉伯国王大学科学学院化学系沙特阿拉伯利雅得11451

CO_2是廉价的Cl源,同时具有无毒、储量丰富的优点,符合绿色化学发展要求.利用CO_2构筑新的C-C键是化学固定CO_2的重要方法.β,γ-不饱和酯类结构单元是许多生物活性分子的重要组成部分,经由双π-烯丙基钯中间体与CO_2反应,合成新的β,γ... 详细信息

CO_2是廉价的Cl源,同时具有无毒、储量丰富的优点,符合绿色化学发展要求.利用CO_2构筑新的C-C键是化学固定CO_2的重要方法.β,γ-不饱和酯类结构单元是许多生物活性分子的重要组成部分,经由双π-烯丙基钯中间体与CO_2反应,合成新的β,γ-不饱和酯类化合物,具有重要意义.CO_2与有机硼化合物的羧化反应己有报道,有机硼化合物具有低毒、对水不敏感等优点.但是己报道的羧化Suzuki偶联反应存在诸多缺点:(1)需要使用含膦或者氮杂环卡宾配体的催化剂,而这些催化剂的制备过程使前期实验步骤变得冗长,同时反应液的酸化后处理过程也会造成环境污染;(2)有机硼试剂的官能团兼容范围窄,限制了底物范围的拓展.本课题组以原位生成的纳米钯粒子为催化剂,在CO_2存在的温和条件下,高效实现了苄氯与烯丙基硼酸频哪醇酯的羧化Suzuki偶联反应.反应过程中无其它配体加入,反应结束后不需要酸化或酯化的后处理过程.该反应将具有广泛的官能团兼容性.本文以TBAB稳定的纳米钯粒子为催化剂,在温和条件下,实现了氯甲基芳香化合物、烯丙基硼酸频哪醇酯和CO_2的三组分羧化Suzuki偶联反应.最佳反应条件为:Pd(acac)_2(5mol%)、TBAB(0.7mmol,1.4 equiv.)、KF(1mmol,2.0 equiv.)、苄基卤代物(0.5 mmol)、烯丙基硼酸频哪醇酯(0.6 mmol,1.2 equiv.)、CO_2(2.0 MPa)、溶剂THF(5 mL),50℃反应24h.在最佳反应条件下,苯环、萘环以及杂芳环的氯甲基化合物均可发生该羧化反应.苯环上取代基的位置对产物的收率有影响.当使用1-溴甲基萘作为底物时反应也能够发生,收率与1-氯甲基萘作为底物时的收率相当.与已报道有机硼试剂的羧化反应相比,该反应体系无需加入配体,原位生成了纳米钯粒子,避免了催化剂或者配体的复杂制备过程.该反应中,氟离子的存在是必要的,对烯丙基硼酸频哪醇酯具有活化作用.

关键词：纳米钯羧化Suzuki偶联二氧化碳苄基氯代物烯丙基硼酸频哪醇酯

Difference of Curcumin Content in Curcuma longa L. (Zingiberaceae) Caused by Hybridization with Other Curcuma Species

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American Journal of Plant Sciences 2011年第2期2卷 111-119页

作者： Hiroshi Hayakawa Yukio Minaniya Katsura Ito yoshinori yamamoto Tatsuya Fukuda 不详

Curcumin, which is traditionally known to have effects on various types of diseases in humans, is found in Curcuma longa L. Previous reports have indicated that the curcumin content varies between the different lines of this species. To clarify the differences in the amounts of curcumin between the lines, we investigated the outcomes of cultivation ex-periments with the hybridization or introgression between C. longa and other Curcuma species using the matK gene of chloroplast DNA (cpDNA) and the external transcribed spacer (ETS) of nuclear DNA (nrDNA). The results show that there is heterogeneity of the ETS and incongruence between the matK and the ETS phylogenetic trees, suggesting that hybridization and introgression had taken place in the diversification of the various lines of C. longa. Moreover, al-though all of the lines had the same cpDNA haplotype of C. longa, the lines of homogeneous C. longa had a high con-tent of curcumin, whereas the lines created by hybridization and introgression with other Curcuma species had a me-dium or low level. These results suggest that the difference of curcumin content among the various lines of C. longa was caused by hybridization and introgression with other Curcuma species.

关键词： Curcuma longa Curcumin Hybridization Introgression Molecular analysis Nuclear DNA

Electrophilic Cyclization of 1-Azido-2-（2-propynyl）benzene to Quinolines

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Electrophilic Cyclization of 1-Azido-2-（2-propynyl）benzene...

Electrophilic Cyclization of 1-Azido-2-（2-propynyl）benzene to Quinolines

第十七届全国金属有机化学学术讨论会

作者： Zhibao Huo Ilya D.Gridnev yoshinori yamamoto Shanghai Jiao Tong University Tohoku University

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Electrophilic Cyclization of 1-Azido-2-（2-propynyl）benzene...

Development of a Molecular Marker to Identify a Candidate Line of Turmeric (Curcuma longa L.) with a High Curcumin Content

第十七届全国金属有机化学学术讨论会

作者：霍志保 Ilya D.Gridnev yoshinori yamamoto School of Environmental Science and Engineering Shanghai Jiao Tong University Department of Chemistry Graduate School of ScienceTohoku University WPI-AIMR (WPI-Advanced Institute for Materials Research) Tohoku University

＜正＞Quinolines represent an important class of alkaloids because of their wide *** quinolines are often found as structural framework in a large number of biologically active natural products and pharmaceuticals.1 Example include anti-Alzheimer agents,anticancer activity,and antimalarial ***,quinoline derivatives have been shown to be outstanding organocatalysts and recognized as useful tools for the

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American Journal of Plant Sciences 2011年第1期2卷 15-26页

作者： Hiroshi Hayakawa Tetsuya Kobayashi Yukio Minaniya Katsura Ito Akira Miyazaki Tatsuya Fukuda yoshinori yamamoto 不详

Dried and fresh rhizomes of the spice turmeric (Curcuma longa L.) are well known in traditional medicine, and curcu- min is widely used in various geographic regions. Although there are differences in the amount of curcumin within this species, identification of the candidate line by rhizome is difficult because of the relative simplicity of its morphological characteristics. To accurately identify lines of C. longa with a high content of curcumin, we analysed several sequences of chloroplast DNA. First, to determine the appropriate outgroup taxa in which to conduct infras-pecific analyses of C. longa, we reconstructed the molecular phylogenetic tree of C. longa and its allied species. The results showed that C. aromatica and C. zedoaria are closely related to C. longa. Next, to develop a molecular marker for identifying lines of C. longa with a high content of curcumin, a network analysis using chloroplast microsatellite regions was performed. Results showed that a unique haplotype within C. longa corresponds to the high curcumin content line. Therefore, the chloroplast microsatellite regions used for the analysis allowed us to determine the lines of this species with high cur- cumin content.

关键词： Chloroplast DNA Curcuma Curcuma Longa Curcumin Molecular Analysis

Changes in Plant Species during Succession in a Sago Forest

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American Journal of Plant Sciences 2014年第24期5卷 3526-3534页

作者： Yoshimasa Kumekawa Matheus Kilmaskossu Makito Mori Akira Miyazaki Katsura Ito Ryo Arakawa Tatsuya Fukuda Hubertus Matanubun yoshinori yamamoto The United Graduate School of Agricultural Science Ehime University Kochi Japan Faculty of Agriculture Kochi University Kochi Japan Papua State University Manokwari Indonesia

The variation in solar environments during succession in sago forests is thought to affect the growth of many plant species. To clarify the pattern of plant colonization in sago forests at various successional stages, we constructed eleven 10 m × 10 m quadrats in different solar conditions in sago forests, measured and calculated the relative illumination intensity, collected all plant species in these quadrats, and used two chloroplast gene sequences—the rbcL gene of ferns and the trnL intron of angiosperms to molecularly identify them. The number of ferns increased while the number of herbaceous species decreased during the process of succession. Moreover, the number of woody species was not significantly correlated with the relative light intensity. Based on these results, it can be concluded that woody species colonized and grew at various successional stages but herbaceous species and ferns did the same in the early and late successional stages, respec-tively, in the sago forest.

关键词： Chloroplast DNA (cpDNA) Plant Species Sago Palm

金或银离子催化的内炔基环丙基硅醚的分子内环化反应

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吉林大学学报（理学版） 2009年第4期47卷 827-831页

作者：刘春丽班大明山本嘉则贵州大学精细化工研究中心贵阳550025 贵州师范大学化学与材料科学学院贵阳550001 日本东北大学大学院理学研究科化学系

在金或银离子的催化下,对7种内炔基环丙基硅醚化合物进行催化环化反应,得到了相应的α,β-不饱和环戊烯基酮的分子内环化产物,最高收率为78%,并通过红外光谱、核磁共振氢谱/碳谱证实了新化合物的结构,提出了环化反应机理.

关键词：金或银离子非端炔基分子内环化反应机理

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纳米多孔金催化有机反应研究进展

分子科学学报 2016年第5期32卷 353-366页

作者：赵玉辉冯秀娟山本嘉则包明大连理工大学精细化工国家重点实验室辽宁大连116024 日本东北大学原子分子材料高等研究所日本仙台980-8577

综述了金纳米多孔材料在催化CO和醇的氧化反应、含不饱和键化合物(炔烃、亚胺和α,β-不饱和醛)的加氢还原反应、炔基芳香醛与炔烃的成环反应、氧化脱氢偶联构筑新C—C键反应和C—X(X=B,Si)键形成反应中的应用研究结果.

关键词：纳米多孔金催化氧化还原 C—C键形成

Profile and removal of endocrine disrupting chemicals by using an ER/AR competitive ligand binding assay and chemical analyses

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Journal of Environmental Sciences 2009年第7期21卷 900-906页

作者： Ze-hua Liu Mamoru Ito yoshinori Kanjo Atsushi yamamoto Department of Urban Engineering Graduate School of Engineering Osaka City University 3-3-138 Sugimoto Sumiyoshi-ku Osaka 558-8585 Japan Osaka City Institute of Public Health and Environmental Sciences 8-34 Tojo-cho Tennoji-ku Osaka 543-0026 Japan

An estrogen receptor （ER）/androgen receptor （AR） ligand competitive binding assay （ER/AR-binding assay） and chemical analyses were used to evaluate the endocrine disrupting chemicals （EDCs） behavior of two municipal wastewater treatment plants （WWTPs）（K and S）. In the influents, estrone （E 1）, androsterone （A）, androstenedione （AD）, BPA （bisphenol A）, NP （nonylphenol） and daidzein （DZ） were detected in high amounts with subsequent 24 h-average concentrations of 350, 1000, 29, 1300, 3900, and 5700 ng/L in K-WWTP and of 310, 620, 59, 1600, 2600, and 8400 ng/L in S-WWTP. The estrogenic （androgenic） activity as 17β-estradiol （E2） equivalents （EEQ） or testosterone （Te） equivalents （TEQ） was consequently 620 ng E2/L （570 ng Te/L） and 580 ng E2/L （800 ng Te/L） for the two WWTPs. The removal efficiencies of the above mentioned sole target chemicals were 51%-100% for K-WWTP and 55.6%-100% for S-WWTP. The removal efficiencies of EEQ were about 73% for both WWTPs, while the removal efficiencies of TEQ were 62.1% for K-WWTP and 98.4% for S-WWTP. In addition, chemical-derived EEQ were about 1.2%-52.4% of those by ER-binding assay for K-WWTP and the corresponding ratios were 1.3%-83.3% for S-WWTP, while chemical derived TEQ were less than 3% of values measured by the AR-binding assay for both WWTPs.

关键词： bioassays ER-binding AR-binding 17β-estradiol equivalents testosterone equivalents