Lin Shanshan, Liu Jianguo, Ma Longlong
CAS Key Laboratory of Renewable Energy, Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou, 510640 People's Republic of China.
University of Chinese Academy of Sciences, Beijing, 100049 People's Republic of China.
Catal Letters. 2023 Jan 20:1-12. doi: 10.1007/s10562-023-04273-7.
Aniline is a group of important platform molecules that has been widely used in the synthesis of other high-value chemicals and pharmaceutical products. How to produce high-value anilines as the high-value chemical intermediates more efficiently and environmentally has always been a research topic in the industry. Catalytic hydrogenation is an environmentally friendly method for preparing halogenated anilines. Traditional noble metal catalysts face the problems of cost and noble metals residue. To improve the purity of the product as well as the activity and recyclability of the catalyst, we prepared a Pd/Fe magnetic bimetallic catalyst supported on N-doped carbon materials to reduce nitrobenzene to aniline under mild conditions. The catalyst has a low Pd loading of 2.35%. And the prepared bimetallic Pd/Fe@N/C catalyst showed excellent catalytic reactivity with the nitrobenzene conversion rate of 99%, and the aniline selectivity of 99% under mild reaction conditions of 0.8 MPa H and 40 °C. A variety of halogenated and aliphatic nitro compounds were well tolerated and had been transformed to the corresponding target amine products with excellent selectivity. In addition, the novel N-doped graphene-encapsulated bimetallic magnetic Pd/Fe@N/C catalyst not only had magnetic physical properties, which was easy to separate, recover, and used for the recycling of the catalyst without metal leaching but also catalyzed highly selective reductive amination of aromatics was a green, economical and environmentally friendly reaction with the only by-product of HO.
The online version contains supplementary material available at 10.1007/s10562-023-04273-7.
苯胺是一类重要的平台分子，已广泛应用于其他高价值化学品和药品的合成。如何更高效、更环保地生产作为高价值化学中间体的高价值苯胺一直是该行业的研究课题。催化氢化是制备卤代苯胺的一种环境友好方法。传统的贵金属催化剂面临成本和贵金属残留问题。为了提高产品纯度以及催化剂的活性和可回收性，我们制备了一种负载在氮掺杂碳材料上的Pd/Fe磁性双金属催化剂，用于在温和条件下将硝基苯还原为苯胺。该催化剂的钯负载量低至2.35%。制备的双金属Pd/Fe@N/C催化剂在0.8 MPa氢气和40℃的温和反应条件下表现出优异的催化活性，硝基苯转化率为99%，苯胺选择性为99%。各种卤代和脂肪族硝基化合物都能被良好耐受，并以优异的选择性转化为相应的目标胺产物。此外，新型的氮掺杂石墨烯包裹的双金属磁性Pd/Fe@N/C催化剂不仅具有磁性物理性质，易于分离、回收且用于催化剂循环使用时无金属浸出，而且催化芳烃的高选择性还原胺化反应是一种绿色、经济且环境友好的反应，唯一的副产物是水。
在线版本包含可在10.1007/s10562-023-04273-7获取的补充材料。
