High Coverage CO Adsorption on Fe6O6 Cluster Using GGA plus U

被引：6
作者：
Yu, Xiaohu [1 ]
Jin, Lingxia [1 ]
Zhao, Caibin [1 ]
Liu, Zhong [2 ]
机构：
[1] Shaanxi Univ Technol, Sch Chem & Environm Sci, Inst Theoret & Computat Chem, Shaanxi Key Lab Catalysis, Hanzhong 723000, Peoples R China
[2] Chinese Acad Sci, Qinghai Inst Salt Lakes, Key Lab Salt Lake Resources & Chem, Xining 810008, Peoples R China
来源：
JOURNAL OF CLUSTER SCIENCE | 2020年 / 31卷 / 03期
基金：
中国国家自然科学基金; 美国国家科学基金会;
关键词：
DFT plus U; CO; Water-gas shift reaction; Fe6O6; Fischer-Tropsch synthesis; Adsorption; IRON-OXIDE CLUSTERS; DENSITY-FUNCTIONAL THEORY; TOTAL-ENERGY CALCULATIONS; WATER-ADSORPTION; FORMATION MECHANISMS; HYDROGEN ADSORPTION; OXIDATION; SURFACES; FE3O4; 1ST-PRINCIPLES;
D O I：
10.1007/s10876-018-1485-0
中图分类号：
O61 [无机化学];
学科分类号：
070301 ; 081704 ;
摘要：
The adsorption of CO molecules on Fe6O6 cluster was systematically studied at different coverage by GGA + U calculations and atomic thermodynamics. Starting from single CO molecule adsorption on Fe6O6 cluster, we have varied the concentration and configuration of CO molecules. It has been found that one surface iron atom of Fe6O6 cluster can coadsorb two CO molecules which can be explained well by the spatial effect. The phase diagrams show that twelve CO molecules binding on Fe6O6 cluster is favorable thermodynamically. It has been found that six CO molecules binding on Fe6O6 cluster is the saturation adsorption according to the stepwise adsorption energy, and the different adsorption states can coexist for two-CO molecules binding on Fe6O6 cluster at high temperature according to probability distribution plot. The adsorption mechanism of CO on Fe6O6 cluster was analyzed by the projected density of states and compared with Fe3O4 surfaces and other small iron oxide clusters.
引用
收藏
页码：591 / 600
页数：10
相关论文
共 77 条
[1]   BAND THEORY AND MOTT INSULATORS - HUBBARD-U INSTEAD OF STONER-I [J].
ANISIMOV, VI ;
ZAANEN, J ;
ANDERSEN, OK .
PHYSICAL REVIEW B, 1991, 44 (03) :943-954
[2]   Charge-ordered insulating state of Fe3O4 from first-principles electronic structure calculations [J].
Anisimov, VI ;
Elfimov, IS ;
Hamada, N ;
Terakura, K .
PHYSICAL REVIEW B, 1996, 54 (07) :4387-4390
[3]   Stability and Metastability of Clusters in a Reactive Atmosphere: Theoretical Evidence for Unexpected Stoichiometries of MgMOx [J].
Bhattacharya, Saswata ;
Levchenko, Sergey V. ;
Ghiringhelli, Luca M. ;
Scheffler, Matthias .
PHYSICAL REVIEW LETTERS, 2013, 111 (13)
[4]   Subsurface cation vacancy stabilization of the magnetite (001) surface [J].
Bliem, R. ;
McDermott, E. ;
Ferstl, P. ;
Setvin, M. ;
Gamba, O. ;
Pavelec, J. ;
Schneider, M. A. ;
Schmid, M. ;
Diebold, U. ;
Blaha, P. ;
Hammer, L. ;
Parkinson, G. S. .
SCIENCE, 2014, 346 (6214) :1215-1218
[5]   IMPROVED TETRAHEDRON METHOD FOR BRILLOUIN-ZONE INTEGRATIONS [J].
BLOCHL, PE ;
JEPSEN, O ;
ANDERSEN, OK .
PHYSICAL REVIEW B, 1994, 49 (23) :16223-16233
[6]   Synthesis of the Highly Reduced [Fe6C(CO)15]4- Carbonyl Carbide Cluster and Its Reactions with H+ and [Au(PPh3)]+ [J].
Bortoluzzi, Marco ;
Ciabatti, Iacopo ;
Cesari, Cristiana ;
Femoni, Cristina ;
Iapalucci, Maria Carmela ;
Zacchini, Stefano .
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY, 2017, (25) :3135-3143
[7]   Density functional theory study of CO adsorption on Fe5C2(001), -(100), and -(110) surfaces [J].
Cao, DB ;
Zhang, FQ ;
Li, YW ;
Jiao, HJ .
JOURNAL OF PHYSICAL CHEMISTRY B, 2004, 108 (26) :9094-9104
[8]   CO ligands stabilize metal chalcogenide Co6Se8(CO)n clusters via demagnetization [J].
Chauhan, Vikas ;
Reber, Arthur C. ;
Khanna, Shiv N. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2017, 19 (47) :31940-31948
[9]   CO Oxidation by Group 3 Metal Monoxide Cations Supported on [Fe(CO)4]2- [J].
Chi, Chaoxian ;
Qu, Hui ;
Meng, Luyan ;
Kong, Fanchen ;
Luo, Mingbiao ;
Zhou, Mingfei .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (45) :14096-14101
[10]   Preparation and Characterization of Uranium-Iron Triple-Bonded UFe(CO)3- and OUFe(CO)3- Complexes [J].
Chi, Chaoxian ;
Wang, Jia-Qi ;
Qu, Hui ;
Li, Wan-Lu ;
Meng, Luyan ;
Luo, Mingbiao ;
Li, Jun ;
Zhou, Mingfei .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (24) :6932-6936
12345678