Understanding the dehydrogenation mechanism over iron nanoparticles catalysts based on density functional theory  

作　　者：Wenjuan Yang Yating Zhu Junjun Li Zheng Chen Farhat Nosheen Qitao Zhang Zhicheng Zhang 

机构地区：[1]SZU-NUS Collaborative Innovation Center for Optoelectronic Science£/Technology,International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education,Institute of Microscale Optoelectronics,Shenzhen University,Shenzhen 518060,China [2]Tianjin Key Laboratory of Molecular Optoelectronic Sciences,Department of Chemistry,School of Science,Tianjin University&Collaborative Innovation Center of Chemical Science and Engineering,Tianjin 300072,China [3]Hanshan Normal University,Chaozhou 521041,China [4]Key Laboratory of Functional Molecular Solids,Ministry of Education,Anhui Key Laboratory of Molecule-Based Materials,College of Chemistry and Materials Science,Anhui Normal University,Wuhu 241000,China [5]Department of Chemistry,Division of Science&Technology,University of Education,Lahore,Pakistan

出　　处：《Chinese Chemical Letters》2021年第1期286-290,共5页中国化学快报（英文版）

基　　金：supported by the National Natural Science Foundation of China(Nos.21866032,21805191);China Postdoctoral Science Foundation(No.2020M672811);the Guangdong Basic and Applied Basic Research Foundation(No.2020A151501982);the“Explorer 100”cluster system of Tsinghua National Laboratory for Information Science and Technology。

摘　　要：The conversion of chemical feedstock materials into high value-added products accompanied with dehydrogenation is of great value in the chemical industry.However,the catalytic dehydrogenation reaction is inhibited by a limited number of expensive noble metal catalysts and lacks understanding of dehydrogenation mechanism.Here,we report the use of heterogeneous non-noble metal iron nanoparticles(NPs) incorporated mesoporous nitrogen-doped carbon to investigate the dehydrogenation mechanism based on experiment observation and density functional theory(DFT) method.Fe NPs catalyst displays excellent performance in the dehydrogenation of 1,2,3,4-tetrahydroquinoline(THQ)with 100% selectivity and 100% conversion for 10-12 h at room temperature.The calculated adsorption energy implies that THQ prefers to adsorb on Fe NPs as compared with absence of Fe NPs.What is more,the energy barrier of transition state is relatively low,illustrating the dehydrogenation is feasible.This work provides an atomic scale mechanism guidance for the catalytic dehydrogenation reaction and points out the direction for the design of new catalysts.

关 键 词：Dehydrogenation mechanism Fe nanoparticles Density functional theory Transition states 1 2 3 4-Tetrahydroquinoline Theoretical calculations 

分 类 号：TQ426[化学工程]