Understanding the dehydrogenation mechanism over iron nanoparticles catalysts based on density functional theory
Understanding the dehydrogenation mechanism over iron nanoparticles catalysts based on density functional theory
复制标题
基于密度泛函理论理解铁纳米粒子催化剂的脱氢机理
DOI：
10.1016/j.cclet.2020.10.040
复制
发表时间：
2021
影响因子：
9.1
通讯作者：
Zhang Zhicheng
中科院分区：
文献类型：
--
作者：
Yang Wenjuan;Zhu Yating;Li Junjun;Chen Zheng;Nosheen Farhat;Zhang Qitao;Zhang Zhicheng
在化学工业中，伴随脱氢将化学原料转化为高附加值产品具有重要价值。然而，催化脱氢反应受到数量有限的昂贵贵金属催化剂的抑制，并且缺乏对脱氢机理的理解。本文基于实验观察和密度泛函理论（DFT）方法，采用非均相非贵金属铁纳米粒子（NPs）掺杂的介孔氮掺杂碳来研究其脱氢机理。Fe NPs催化剂在1，2，3，4-四氢喹啉（THQ）脱氢反应中表现出优异的性能，在室温下反应10-12 h，选择性和转化率均为100%。计算的吸附能表明，THQ更喜欢吸附在铁纳米粒子相比，没有铁纳米粒子。过渡态的能垒较低，说明脱氢反应是可行的。本工作为催化脱氢反应提供了原子尺度的机理指导，为新型催化剂的设计指明了方向。
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.