Single-atom Fe with Fe 1 N 3 structure showing superior performances for both hydrogenation and transfer hydrogenation o
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Published online 15 October 2020 | https://doi.org/10.1007/s40843-020-1443-8
Single-atom Fe with Fe1N3 structure showing superior performances for both hydrogenation and transfer hydrogenation of nitrobenzene 1†
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Shubo Tian , Min Hu , Qi Xu , Wanbing Gong , Wenxing Chen , Jiarui Yang , Youqi Zhu , 3 2 1 3 1* 1 Chun Chen , Jia He , Qiang Liu , Huijun Zhao , Dingsheng Wang and Yadong Li ABSTRACT The design of non-noble metal heterogeneous catalyst with superior performance for selective hydrogenation or transfer hydrogenation of nitroarenes to amines is significant but challenging. Herein, a single-atom Fe supported by nitrogen-doped carbon (Fe1/N-C) catalyst is reported. The Fe1/N-C sample shows superior performances for the selective hydrogenation and transfer hydrogenation of nitrobenzene to aniline at different temperatures. Density functional theory (DFT) calculations show that the superior catalytic activity for the selective hydrogenation at lower temperatures could be attributed to the effective activation of the reactant and intermediates by the Fe1/N-C. Moreover, the excellent performance of Fe1/N-C for the selective transfer hydrogenation could be attributed to that the reaction energy barrier for dehydrogenation of isopropanol can be overcome by elevated temperatures. Keywords: single-atomic Fe catalyst, hydrogenation of nitrobenzene, transfer hydrogenation, DFT calculations
INTRODUCTION Amines are important chemical intermediates for fine chemicals and pharmaceuticals [1,2]. The selective hydrogenation of nitroarenes to anilines with hydrogen molecules and transfer hydrogenation with organic molecules as the hydrogen donor are extensively utilized
approaches in practical applications [3–11]. Although numerous excellent homogeneous catalysts and noble metal heterogeneous catalysts have been developed for the catalytic conversion of nitroarenes to anilines, the difficulties in the separation and reuse of the homogeneous catalysts and the high cost of the noble metal heterogeneous catalysts hinder their further applications [12–15]. Therefore, it remains a significant challenge to synthesize the non-noble metal catalyst that possesses superior performance for the hydrogenation of nitrobenzene. Iron catalyst is one of the most used nonnoble metal catalysts in the catalytic reaction, which is the best candidate metal for the hydrogenation of nitrobenzene [16–18]. However, the heterogeneous iron catalyst with excellent catalytic performances for both selective hydrogenation and transfer hydrogenation of nitroarenes has seldom been studied. Single-atom catalysis has become one of the most active research frontiers in heterogeneous catalysis due to the uniform active site and total atom utilization efficiency [19–36]. The uniform active site can provide an ideal platform for deeper understanding of the fundamentals. Meanwhile, the total atom utilization efficiency can naturally increase the catalytic performance. It is worth noting that the single-atom catalysts have exhibited excellent pe
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