| 苏玲,张月成,赵继全.树枝状聚酰胺胺负载TEMPO的合成及其催化分子氧氧化醇的性能[J].分子催化,2014,(5):400-409 |
| 树枝状聚酰胺胺负载TEMPO的合成及其催化分子氧氧化醇的性能 |
| Synthesis of dendritic polyamidoamine supported 2, 2, 6, 6-tetramethylpiperidine-1-oxyl and its catalytic performance on the oxidation of alcohols with molecular oxygen as oxidant |
| 投稿时间：2014-06-11 修订日期：2014-07-04 |
| DOI： |
| 中文关键词: 树枝状 聚酰胺胺（PAMAM） 2,2,6,6-四甲基哌啶氮氧自由基（TEMPO） 醇氧化 分子氧 |
| 英文关键词:dendritic, polyamidoamine (PAMAM), 2, 2, 6, 6-tetramethylpiperidine-1-oxyl (TEMPO), alcohol oxidation, molecular oxygen |
| 基金项目:国家自然科学基金项目（面上项目，重点项目，重大项目） |
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| 中文摘要: |
| 以乙二胺和丙烯酸甲酯为原料经重复Michael和酯氨解反应制备出二代（2.0 G）树枝状聚酰胺胺（PAMAM）。PAMAM与2,2,6,6-四甲基哌啶酮氮氧自由基经缩合、还原将PAMAM与2,2,6,6-四甲基哌啶氮氧自由基（TEMPO）键连，得到PAMAM负载的TEMPO（PAMAM-TEMPO）。采用1H NMR、13C NMR以及FT-IR等手段对中间体及最终产物进行了表征。将PAMAM-TEMPO与CuBr2以及2,2-联吡啶结合构成催化体系,用于分子氧为氧化剂的醇的选择性氧化反应，结果表明该体系对苄基以及烯丙基伯醇的氧化显示出良好的催化活性和选择性。结果还证明，TEMPO的负载使氧化产物醛很容易与催化体系分离，而且催化剂可以循环使用。 |
| 英文摘要: |
| A second-generation dendritic polyamidoamine (PAMAM) was prepared via repeated Michael addition and aminolysis of ethylenediamine and methyl acrylate. The obtained PAMAM condensed with 4-oxo-2, 2, 6, 6-tetramethylpiperidinooxy followed by reduction to afford a PAMAM supported 2, 2, 6, 6-tetramethylpiperidine-1-oxyl (PAMAM-TEMPO). The PAMAM-TEMPO and the intermediates in the preparation of it were characterized by 1H NMR, 13C NMR and FT-IR. The PAMAM-TEMPO in combination with CuBr2 and 2, 2’-bipyridine as a catalytic system was applied to the selective oxidation of alcohols with molecular oxygen as an oxidant, and showed high activity and selectivity in oxidation of benzyl alcohols and allyl alcohols. The immobilization of TEMPO on PAMAM allowed easy separation of the oxidation products (aldehydes) from the catalytic system, and the recovered catalyst can be recycled for several times directly. |
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