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负载钌的磁铁矿作为一种可回收的催化剂,用于醇类作为亲电试剂的氢转移过程中胺类、磺胺类、亚磺酰胺类和硝基芳烃的 N-烷基化反应。

Impregnated ruthenium on magnetite as a recyclable catalyst for the N-alkylation of amines, sulfonamides, sulfinamides, and nitroarenes using alcohols as electrophiles by a hydrogen autotransfer process.

机构信息

Instituto de Síntesis Orgánica (ISO), Facultad de Ciencias, Universidad de Alicante, Alicante, Spain.

出版信息

J Org Chem. 2011 Jul 15;76(14):5547-57. doi: 10.1021/jo200559h. Epub 2011 Jun 16.

Abstract

Various impregnated metallic salts on magnetite have been prepared, including cobalt, nickel, copper, ruthenium, and palladium salts, as well as a bimetallic palladium-copper derivative. Impregnated ruthenium catalyst is a versatile, inexpensive, and simple system for the selective N-monoalkylation of amino derivatives with poor nucleophilic character, such as aromatic and heteroaromatic amines, sulfonamides, sulfinamides, and nitroarenes, using in all cases alcohols as the initial source of the electrophile, through a hydrogen autotransfer process. In the case of sulfinamides, this is the first time that these amino compounds have been alkylated following this strategy, allowing the use of chiral sulfinamides and secondary alcohols to give the alkylated compound with a diastereomeric ratio of 92:8. In these cases, after alkylation, a simple acid deprotection gave the expected primary amines in good yields. The ruthenium catalyst is quite sensitive, and small modifications of the reaction medium can change the final product. The alkylation of amines using potassium hydroxide renders the N-monoalkylated amines, and the same protocol using sodium hydroxide yields the related imines. The catalyst can be easily removed by a simple magnet and can be reused up to ten times, showing the same activity.

摘要

已经制备了各种浸渍在磁铁矿上的金属盐,包括钴、镍、铜、钌和钯盐,以及一种双金属钯-铜衍生物。浸渍钌催化剂是一种多功能、廉价且简单的系统,可用于选择性地对具有较差亲核性的氨基衍生物进行 N-单烷基化,如芳族和杂芳族胺、磺胺、亚磺酰胺和硝基芳烃,在所有情况下均使用醇作为亲电试剂的初始来源,通过氢自动转移过程。对于亚磺酰胺,这是首次使用该策略对这些氨基化合物进行烷基化,允许使用手性亚磺酰胺和仲醇来获得非对映体比例为 92:8 的烷基化化合物。在这些情况下,烷基化后,通过简单的酸脱保护可得到良好收率的预期伯胺。钌催化剂非常灵敏,反应介质的微小变化可以改变最终产物。使用氢氧化钾进行胺的烷基化可得到 N-单烷基化的胺,而使用氢氧化钠的相同方案则得到相关的亚胺。催化剂可以通过简单的磁铁轻松去除,并可重复使用多达十次,保持相同的活性。

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