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Formation Mechanism, Geometric Stability and Catalytic Activity of a Single Iron Atom Supported on N‐Doped Graphene
Author(s) -
Tang Yanan,
Chen Weiguang,
Wu Bingjie,
Zhao Gao,
Liu Zhiyong,
Li Yi,
Dai Xianqi
Publication year - 2019
Publication title -
chemphyschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.016
H-Index - 140
eISSN - 1439-7641
pISSN - 1439-4235
DOI - 10.1002/cphc.201900666
Subject(s) - graphene , catalysis , density functional theory , chemistry , molecule , doping , atom (system on chip) , computational chemistry , photochemistry , chemical engineering , materials science , nanotechnology , organic chemistry , optoelectronics , computer science , engineering , embedded system
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/O 2 and CO/O 2 molecules 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→2CO 2 +N 2 ) 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.