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Au/MOF催化剂的制备、表征及其催化三组分偶联反应
  • ISSN号:0253-9837
  • 期刊名称:《催化学报》
  • 时间:0
  • 分类:O[理学]
  • 作者机构:[1]中国石油大学(北京)化工学院重质油国家重点实验室,北京102249
  • 相关基金:国家自然科学基金(20903119 21173269); 教育部新世纪优秀人才支持计划
中文摘要:

采用后合成共价修饰法和一锅法分别制备了催化剂IRMOF-3-SI-Au(PS)和IRMOF-3-SI-Au(OP),运用X射线衍射、红外光谱、热重-差热分析、透射电镜以及程序升温还原对催化剂进行了表征,探索了这两种催化剂在醛、炔和胺三组分偶联反应中的催化性能,并推测了可能的反应机理.结果表明,两种催化剂对醛、炔和胺三组分偶联反应均具有较高的催化活性,产物炔丙基胺类选择性为100%,且可循环使用;结晶度较低的IRMOF-3-SI-Au(PS)的活性高于结晶度较高的IRMOF-3-SI-Au(OP);催化剂对芳香醛和脂肪醛以及环状胺均具有较高的催化活性,且对带有吸电子基团的芳香醛的活性高于带有供电子基团的.

英文摘要:

IRMOF-3-SI-Au(PS) and IRMOF-3-SI-Au(OP) catalysts were synthesized by post-synthesis method(PS) and one-pot method(OP),respectively.The catalysts were characterized by X-ray diffraction,infrared spectroscopy,thermogravimetric analysis and differential thermal,transmission electron microscopy,and temperature-programmed reduction.These two catalysts were tested by three-component coupling reaction of aldehydes,alkynes,and amines.The substrate scope,catalyst reusability,and possible mechanism were investigated.Both two catalysts showed higher conversions of benzaldehyde and 100% selectivity for propargylamines.Compared with IRMOF-SI-Au(OP),IRMOF-SI-Au(PS) gave a higher aldehyde consumption rate at 120 oC(13.7 vs 2.0 mmol/(g.h)) based on total gold content.Both aromatic and aliphatic aldehydes including those bearing functional groups,such as alkoxy,alkyl,and chloro-group,were able to undergo the corresponding three-component-coupling.It was found that aryl aldehydes possessing electron-drawing group afforded higher conversion than that with an electron-donating group bound to the benzene ring.Among the various amines tested,alicyclic amines,such as piperidine,pyrolidine,and morpholine,gave high conversions of benzaldehyde,whereas the diethylamine afforded lower conversion of benzaldehyde.The catalysts could be reused for three reaction cycles with only slight drop in activity.A tentative mechanism was proposed involving the activation of the C-H bond of alkyne by IRMOF-3 immobilized gold catalysts.

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期刊信息
  • 《催化学报》
  • 北大核心期刊(2011版)
  • 主管单位:中国科学院
  • 主办单位:中国化学会 中国科学院大连化学物理研究所
  • 主编:李灿 张涛
  • 地址:大连市沙河口区中山路457号
  • 邮编:116023
  • 邮箱:chxb@dicp.ac.cn
  • 电话:0411-84379240
  • 国际标准刊号:ISSN:0253-9837
  • 国内统一刊号:ISSN:21-1195/O6
  • 邮发代号:8-93
  • 获奖情况:
  • 第三届国家期刊奖提名奖,中国科协精品科技期刊示范项目
  • 国内外数据库收录:
  • 俄罗斯文摘杂志,美国化学文摘(网络版),荷兰文摘与引文数据库,美国工程索引,美国剑桥科学文摘,美国科学引文索引(扩展库),日本日本科学技术振兴机构数据库,中国中国科技核心期刊,中国北大核心期刊(2004版),中国北大核心期刊(2008版),中国北大核心期刊(2011版),中国北大核心期刊(2014版),英国英国皇家化学学会文摘,中国北大核心期刊(2000版)
  • 被引量:19199