Formation Mechanism, Geometric Stability and Catalytic Activity of a Single Iron Atom Supported on N-Doped Graphene
Formation Mechanism, Geometric Stability and Catalytic Activity of a Single Iron Atom Supported on N-Doped Graphene
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N掺杂石墨烯负载单铁原子的形成机制、几何稳定性和催化活性
DOI：
10.1002/cphc.201900666
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发表时间：
2019
期刊：
影响因子：
2.9
通讯作者：
Dai Xianqi
中科院分区：
文献类型：
--
作者：
Tang Yanan;Chen Weiguang;Wu Bingjie;Zhao Gao;Liu Zhiyong;Li Yi;Dai Xianqi
基于密度泛函理论(DFT)计算，系统研究了xN掺杂石墨烯(xN-石墨烯-Fe，x=1，2，3)单原子铁的形成构型、稳定性和催化性能。研究发现，不同种类和数量的气体反应物可以有效地调节3 N-石墨烯-Fe体系的电子结构和磁性。对于NO和CO氧化反应，对比分析了NO/O2和CO/O2分子在反应底物上的共吸附构型。通过朗缪尔-辛舍伍德(L H)和Eley-R理想(ER)机制进行的NO氧化反应比CO氧化反应具有相对较小的能垒。相比之下，预吸附的2NO与2CO分子(2NO+2CO→2CO2+N2)通过电流变反应(<；0.4 eV)反应在能量上更有利。这些结果可为NO和CO氧化的理论研究和石墨烯类有毒气体脱除催化剂的设计提供有益的参考。
Based on density functional theory (DFT) calculations, the formation geometries, stability and catalytic properties of single‐atom iron anchored on xN‐doped graphene (xN‐graphene‐Fe, x=1, 2, 3) sheet are systemically investigated. It is found that the different kinds and numbers of gas reactants can effectively regulate the electronic structure and magnetic properties of the 3 N‐graphene‐Fe system. For NO and CO oxidation reactions, the coadsorption configurations of NO/O2and CO/O2molecules on a reactive substrate as the initial state are comparably analyzed. The NO oxidation reactions through the Langmuir–Hinshelwood (LH) and Eley‐Rideal (ER) mechanisms have relatively smaller energy barriers than those of the CO oxidation processes. In comparison, the preadsorbed 2NO reacting with 2CO molecules (2NO+2CO→2CO2+N2) through ER reactions (<0.4 eV) are energetically more favorable processes. These results can provide beneficial references for theoretical studies on NO and CO oxidation and designing graphene‐based catalyst for toxic gas removal.