The high-value transformation of nitrogen-containing compounds through a facile, cost-effective, and eco-friendly one-pot strategy holds significant importance. However, this process typically involves the use of metal catalysts and is limited by low activity as well as the requirement of high temperature and pressure. Herein, we describe a general and efficient metal-free N-doped mesoporous carbon material using well-defined ligand 1,10-phenanthroline as the precursor and silica colloid as the hard template. Formic acid is both a reducing agent and a formylation reagent, and structurally distinct mono- or multi-substituted nitroarenes and quinolines can be selectively N-formylation in a one-pot method. The catalyst can be easily recovered without observable loss of efficiency for ten consecutive uses. The control experiments and density functional theory (DFT) calculations indicate that formic acid mainly obtains active hydrogen in the form of O–H bond cleavage, which benefits from the strong adsorption and enhanced activity generated by the interaction between graphitic nitrogen species in the catalyst and formic acid. The excellent catalytic performance of the meso-phen-X catalyst is attributed to the synergistic effect of graphitic N and large specific surface area, providing a promising method for the development of non-metallic catalyst-modified carbon materials.

中文翻译：

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可重复使用的无金属介孔碳催化的硝基芳烃和喹啉的还原 N-甲酰化


通过简单、经济高效且环保的一锅法对含氮化合物进行高价值转化具有重要意义。然而，这个过程通常涉及金属催化剂的使用，并且受到低活性以及高温和高压要求的限制。在本文中，我们描述了一种通用且高效的无金属 N 掺杂介孔碳材料，使用定义明确的配体 1,10-菲咯啉作为前驱体，二氧化硅胶体作为硬模板。甲酸既是还原剂又是甲酰化试剂，结构不同的单取代或多重取代的硝基芳烃和喹啉可以在一锅法中选择性地进行 N-甲酰化。催化剂可以很容易地回收，而不会在连续十次使用时出现明显的效率损失。控制实验和密度泛函理论 （DFT） 计算表明，甲酸主要以 O-H 键裂解的形式获得活性氢，这得益于催化剂中石墨氮物种与甲酸相互作用产生的强吸附和增强活性。meso-phen-X 催化剂优异的催化性能归因于石墨 N 和大比表面积的协同作用，为非金属催化剂改性碳材料的开发提供了一种有前途的方法。