Shedding light on the reversible deactivation of carbon-supported single-atom catalysts in hydrogenation reaction  

作　　者：Runze Chen Xiaoying Wang Jianfei Dang Songjie Yun Liqiang Wang Fangong Kong You-Nian Liu 

机构地区：[1]State Key Laboratory of Biobased Material and Green Papermaking,Qilu University of Technology,Jinan 250353,China [2]School of Material Science and Engineering,Zhengzhou University,Zhengzhou 450001,China [3]School of Chemical Engineering,Zhengzhou University,Zhengzhou 450001,China [4]Hunan Provincial Key Laboratory of Micro&Nano Materials Interface Science,College of Chemistry and Chemical Engineering,Central South University,Changsha 410083,China

出　　处：《Nano Research》2024年第6期4807-4814,共8页纳米研究（英文版）

基　　金：the National Natural Science Foundation of China(Nos.22008221 and 22238013);the Foundation of State Key Laboratory of Biobased Material and Green Papermaking,Qilu University of Technology,Shandong Academy of Sciences(No.GZKF202010).

摘　　要：Carbon-supported single-atom catalysts were found to suffer reversible deactivation in catalytic hydrogenation,but the mechanism is still unclear.Herein,nitro compounds hydrogenation catalyzed by N-doped carbon-supported Co single atom(Co1/NC)was taken as a model to uncover the mechanism of the reversible deactivation phenomenon.Co1/NC exhibited moderate adsorption towards the substrate molecules(i.e.,nitro compounds or related intermediates),which could be strengthened by the confinement effect from the porous structure.Consequently,substrate molecules tend to accumulate within the pore channel,especially micropores that host Co1,making it difficult for the reactants to access the active sites and finally leading to their deactivation.The situation could be even worse when the substrate molecules possess a large size.Nevertheless,the catalytic activity of Co1/NC could be restored via a simple thermal treatment,which could remove the adsorbates within the pore channel,hence releasing active sites that were originally inaccessible to reactants.

关 键 词：single-atom catalysts porous carbon support reversible deactivation mechanistic study hydrogenation reaction 

分 类 号：O64[理学—物理化学]