Single-atomic-site iron on N-doped carbon for chemoselective reduction of nitroarenes  

作　　者：Guoping Lu Kangkang Sun Yamei Lin Qixuan Du Jiawei Zhang Kui Wang Pengcheng Wang 

机构地区：[1]School of Chemical Engineering,Nanjing University of Science&Technology,Nanjing 210094,China [2]Institute of Chemical Industry of Forest Products,Chinese Academy of Forestry,National Engineering Laboratory for Biomass Chemical Utilization,Nanjing 210042,China [3]School of Food Science and Pharmaceutical Engineering,Nanjing Normal University,Nanjing 210032,China [4]College of Materials Science and Engineering,Hunan University,Changsha 410082,China

出　　处：《Nano Research》2022年第1期603-611,共9页纳米研究（英文版）

基　　金：the Fundamental Research Funds for the Central Universities(No.30920021120);the Key Laboratory of Biomass Energy and Material,Jiangsu Province(No.JSBEM201912);the National Natural Science Foundation of China(No.21905089);the Chinese Postdoctoral Science Foundation(No.2019M662775)for financial support。

摘　　要：A facile,gram-scale and sustainable approach has been established for the synthesis of single-atomic-site iron on N-doped carbon(Fe_(SA)@NC-20A)via the pyrolysis of aniline modified FeZn-ZIFs,in which the synthesis of zeolitic imidazolate frameworks(ZIFs)can be accomplished in water at room temperature,and no acid etching is required.The as-synthesized catalyst exhibits better performance on the chemoselective hydrogenation of nitroarenes with a broad substrate scope(turnover frequency(TOF)up to 1,727 h^(-1),23 examples)than most of previously reported works.Based on high-angle annular dark field scanning transmission microscopy(HAADF-STEM)images in combination with X-ray photoelectron spectroscopy(XPS),X-ray absorption spectroscopy(XAS),electron spin resonance(ESR),and Mossbauer spectroscopy,Fe is dispersed as single atoms via forming FeNx(x=4-6).This work not only determines the active sites of FesA@NC-20A for hydrogenation(FeN4),but also proposes tentative pathways for both N-H activation of hydrazine and the reduction of nitroarene on FeN4 site,both of which are the key steps for the hydrogenation of nitroarenes.In addition,this catalyst shows excellent stability,and no significant activity degradation is observed when recycling for 10 times or restoring in air for 2 months.

关 键 词：single-atom-site iron zeolitic imidazolate framework the hydrogenation of nitroarene N-doped carbon drug synthesis 

分 类 号：O62[理学—有机化学]