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纳米介孔Ru-PPh2-SBA-16催化水相中高烯丙醇异构化反应的研究
  • ISSN号:0251-0790
  • 期刊名称:《高等学校化学学报》
  • 时间:0
  • 分类:O643[理学—物理化学;理学—化学]
  • 作者机构:[1]上海师范大学化学系,上海200234
  • 相关基金:国家自然科学基金(批准号:20377031,20407014)资助.
中文摘要:

以2-(二苯基膦)乙基三乙氧基硅烷和正硅酸乙酯为混合硅源,采用延时共缩聚法经表面活性剂F127自组装合成了二苯基膦(PPh2)修饰的SBA-16纳米介孔分子筛(PPh2-SBA-16),通过PPh2配体络合Ru(Ⅱ)化合物制备出固载化的Ru(Ⅱ)非均相催化剂(Ru-PPh2-SBA-16),样品仍然保持了SBA-16的规整孔道结构.以水相中高烯丙醇异构化反应为探针,考察了所制备催化剂的催化性能,发现其对目标产物具有高选择性,虽然其催化活性略低于对应的均相Ru(Ⅱ)催化剂,但该催化剂易与产物分离,且重复使用三次后催化效率基本不变,活性相与载体结合牢固,不存在明显的脱落和流失,因此更适合于工业化应用.

英文摘要:

Based on the serf-assembly of F127, a new SBA-16-1ike mesoporous silica modified with diphenylphosphine group ( PPh2-SBA-16 ) was synthesized by extend co-condensation with tetraethoxysilane (TEOS) and 2-(diphenylphosphino) ethyltriethoxysilane (DPPTS) as the mixed silicon source. The PPh2-SBA-16 was used as a support to immobilize the Ru ( Ⅱ ) ions through strong coordination between PPh2-group and Ru( Ⅱ ), denoted as Ru-PPh2-SBA-16. The characterizations demonstrate that the Ru-PPh2-SBA-16 still remained ordered mesoporous structure. During the isomerization of homoallylic alcohols carried in water as a environmentally friendly medium, the as-prepared Ru-PPh2-SBA-16 catalyst exhibited an excellent selectivity, almost the same as the corresponding homogeneous catalyst [ RuCl2 ( PPh3 ) 3 ]. Although its activity was slightly lower than that of RuCl2 (PPh3)3, the Ru-PPh2-SBA-16 could be considered more suitable for industrial application based on the following benefits : ( 1 ) The catalyst could be easily separated from the reaction products. (2) The catalyst could be used repetitively at least for 3 times without significant activity decrease. (3) The Ru( Ⅱ ) was strongly immobilized on the support which could effectively inhibit the leaching of active sites and protect the environmental pollution from heavy metals.

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期刊信息
  • 《高等学校化学学报》
  • 北大核心期刊(2011版)
  • 主管单位:中华人民共和国教育部
  • 主办单位:吉林大学 南开大学
  • 主编:周其凤
  • 地址:吉林大学南胡校区
  • 邮编:130012
  • 邮箱:cjcu@jlu.edu.cn
  • 电话:0431-88499216
  • 国际标准刊号:ISSN:0251-0790
  • 国内统一刊号:ISSN:22-1131/O6
  • 邮发代号:12-40
  • 获奖情况:
  • 首届及第二届国家期刊奖,连续两届“百种中国杰出学术期刊”,中国期刊方阵“双高”期刊
  • 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:50676