Superhydrophobic nickel/carbon core–shell nanocomposites for the hydrogen transfer reactions of nitrobenzene and N-heterocycles,Green Chemistry

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Superhydrophobic nickel/carbon core–shell nanocomposites for the hydrogen transfer reactions of nitrobenzene and N-heterocycles
Green Chemistry ( IF 9.3 ) Pub Date : 2020/02/18 , DOI: 10.1039/c9gc04358f
Shaofeng Pang _{1,

2,

3,

4,

5} , Yujing Zhang _{4,

6,

7,

8} , Qiong Su _{1,

2,

3,

4,

5} , Fangfang Liu _{1,

2,

3,

4,

5} , Xin Xie _{1,

2,

3,

4,

5} , Zhiying Duan _{1,

2,

3,

4,

5} , Feng Zhou _{4,

9,

10,

11,

12} , Ping Zhang _{1,

2,

3,

4,

5} , Yanbin Wang _{1,

2,

3,

4,

5}

Affiliation

In this work, catalytic hydrogen transfer as an effective, green, convenient and economical strategy is for the first time used to synthesize anilines and N-heterocyclic aromatic compounds from nitrobenzene and N-heterocycles in one step. Nevertheless, how to effectively reduce the possible effects of water on the catalyst by removal of the by-product water, and to further introduce water as the solvent based on green chemistry are still challenges. Since the structures and properties of carbon nanocomposites are easily modified by controllable construction, a one step pyrolysis process is used for controllable construction of micro/nano hierarchical carbon nanocomposites with core–shell structures and magnetic separation performance. Using various characterization methods and model reactions the relationship between the structure of Ni@NCFs (nickel–nitrogen-doped carbon frameworks) and catalytic performance was investigated, and the results show that there is a positive correlation between the catalytic performance and hydrophobicity of catalysts. Besides, the possible catalytically active sites, which are formed by the interaction of pyridinic N and graphitic N in the structure of nitrogen-doped graphene with the surfaces of Ni nanoparticles, should be pivotal to achieving the relatively high catalytic performance of materials. Due to its unique structure, the obtained Ni@NCF-700 catalyst with superhydrophobicity shows extraordinary performances toward the hydrogen transfer reaction of nitrobenzene and N-heterocycles in the aqueous state; meanwhile, it was also found that Ni@NCF-700 still retained its excellent catalytic activity and structural integrity after three cycles. Compared with traditional catalytic systems, our catalytic systems offer a highly effective, green and economical alternative for nitrobenzene and N-heterocycle transformation, and may open up a new avenue for simple construction of structure and activity defined carbon nanocomposite heterogeneous catalysts with superhydrophobicity.

中文翻译：

超疏水镍/碳核-壳纳米复合材料，用于硝基苯和N-杂环的氢转移反应

在这项工作中，催化氢转移作为一种有效，绿色，方便且经济的策略，首次用于一步一步地从硝基苯和N-杂环合成苯胺和N-杂环芳族化合物。然而，如何通过除去副产物水有效地减少水对催化剂的可能影响，以及基于绿色化学进一步引入水作为溶剂仍然是挑战。由于碳纳米复合材料的结构和性质很容易通过可控的结构进行修饰，因此一步式热解工艺可用于具有核壳结构和磁选性能的微米/纳米级碳纳米复合材料的可控结构。使用各种表征方法和模型反应研究了Ni @ NCFs（镍氮掺杂碳骨架）的结构与催化性能之间的关系，结果表明，催化剂的催化性能与疏水性之间存在正相关关系。此外，由氮掺杂石墨烯结构中的吡啶N和石墨N与Ni纳米颗粒的表面相互作用而形成的可能的催化活性位点对于实现材料的较高催化性能至关重要。由于其独特的结构，所获得的具有超疏水性的Ni @ NCF-700催化剂对硝基苯和N-杂环在水态下的氢转移反应表现出非凡的性能。与此同时，还发现Ni @ NCF-700在三个循环后仍保持其优异的催化活性和结构完整性。与传统的催化体系相比，我们的催化体系为硝基苯和N-杂环的转化提供了一种高效，绿色和经济的替代方法，并可能为简单构建结构和活性定义的具有超疏水性的碳纳米复合非均相催化剂开辟新途径。

更新日期：2020-03-24

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