当前位置: X-MOL 学术J. Catal. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
One-pot synthesis of secondary amine via photoalkylation of nitroarenes with benzyl alcohol over Pd/monolayer H1.07Ti1.73O4·H2O nanosheets
Journal of Catalysis ( IF 7.3 ) Pub Date : 2018-03-16 , DOI: 10.1016/j.jcat.2018.02.005
Yujie Song , Hao Wang , Shijing Liang , Yan Yu , Liuyi Li , Ling Wu

The photoalkylation of nitroarenes with benzyl alcohols in one pot at room temperature and 1 atm N2 was achieved over the Pd/H1.07Ti1.73O4·H2O nanosheets. The sample shows efficient photocatalytic activity with high conversion of nitrobenzene (99%) and selectivity of secondary amine (85%). This flexible photocatalytic system is also applicable to other nitroarenes with high efficiency. Results of in situ FTIR, DRS, and in situ ESR revealed that the benzyl alcohol and nitrobenzene molecules can bind with the surface Lewis and Brønsted acid sites in the catalyst via the HO⋯Ti and NO2⋯HOTi species. The formation of surface coordination species results in not only the activation of reactant molecules via surface electron transfer, but also the expanded visible light absorption of the catalyst. Moreover, in situ ESR suggested that the surface coordination can also facilitate the formation of oxygen vacancies in catalysts, which can greatly promote the exposure of Lewis sites and enhance the activation of reactant molecules. Finally, a possible hydrogen transfer strategy over the sample is proposed on a molecular level.



中文翻译:

在Pd /单层H 1.07 Ti 1.73 O 4 ·H 2 O纳米片上通过硝基芳烃与苄醇的光烷基化一锅合成仲胺

在Pd / H 1.07 Ti 1.73 O 4 ·H 2 O纳米片上,在室温和1个atm N 2下,在一个锅中用苄醇对硝基芳烃进行光烷基化。该样品显示出高效的光催化活性,其中硝基苯的转化率高(99%),仲胺的选择性高(85%)。这种灵活的光催化系统还可以高效地应用于其他硝基芳烃。原位FTIR,DRS和原位ESR结果表明,苯甲醇和硝基苯分子可以通过H O⋯Ti和NO 2 ⋯H O与催化剂表面的路易斯酸和布朗斯台德酸键结合钛种。表面配位物质的形成不仅导致通过表面电子转移的反应物分子的活化,而且导致催化剂的扩大的可见光吸收。此外,原位ESR表明表面配位还可以促进催化剂中氧空位的形成,这可以大大促进路易斯位点的暴露并增强反应物分子的活化。最后,在分子水平上提出了样品上可能的氢转移策略。

更新日期:2018-03-16
down
wechat
bug