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Title: First principles density functional theory study of Pb doped α-MnO2 catalytic materials

Abstract

Here, the impact of Pb in the tunnels of manganese oxide octahedral molecular sieves on chemical state of Mn species and lattice oxygen were investigated utilizing density functional theory calculations. The results show that the Pb dopant in the tunnels of OMS-2 could reduce the average valence states of Mn. The lower energy required for bulk oxygen defects formation in Pb-OMS-2 validates the activation of lattice oxygen by inclusion of tunnel dopant. The inclusion of Pb promotes the catalytic oxidation activity of OMS-2 by reducing the energy required for the surface lattice oxygen migration during the Mars – van Krevelen oxidation process.

Authors:
 [1];  [1];  [1];  [1];  [2];  [3];  [4]
  1. Wuhan Inst. of Technology, Wuhan (China). Key Lab. for Green Chemical Process of Ministry of Education and School of Chemical Engineering and Pharmacy
  2. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
  3. Washington State Univ., Pullman, WA (United States). Bioproducts, Sciences and Engineering Lab. and Dept. of Biological Systems Engineering
  4. East China Inst. of Chemical Technology, Shanghai (China). School of Chemical Engineering
Publication Date:
Research Org.:
National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV (United States)
Sponsoring Org.:
USDOE Office of Fossil Energy (FE); Hubei Provincial Natural Science Foundation (China)
OSTI Identifier:
1461404
Grant/Contract Number:  
2013CFA091; 2016CFA079
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Physics Letters
Additional Journal Information:
Journal Volume: 695; Journal Issue: C; Journal ID: ISSN 0009-2614
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Density functional theory; Cryptomelane-type manganese oxides; Pb dopant; Oxygen vacancy; Catalytic oxidation

Citation Formats

Song, Zilin, Yan, Zhiguo, Yang, Xiaojun, Bai, Hang, Duan, Yuhua, Yang, Bin, and Leng, Li. First principles density functional theory study of Pb doped α-MnO2 catalytic materials. United States: N. p., 2018. Web. https://doi.org/10.1016/j.cplett.2018.02.023.
Song, Zilin, Yan, Zhiguo, Yang, Xiaojun, Bai, Hang, Duan, Yuhua, Yang, Bin, & Leng, Li. First principles density functional theory study of Pb doped α-MnO2 catalytic materials. United States. https://doi.org/10.1016/j.cplett.2018.02.023
Song, Zilin, Yan, Zhiguo, Yang, Xiaojun, Bai, Hang, Duan, Yuhua, Yang, Bin, and Leng, Li. Fri . "First principles density functional theory study of Pb doped α-MnO2 catalytic materials". United States. https://doi.org/10.1016/j.cplett.2018.02.023. https://www.osti.gov/servlets/purl/1461404.
@article{osti_1461404,
title = {First principles density functional theory study of Pb doped α-MnO2 catalytic materials},
author = {Song, Zilin and Yan, Zhiguo and Yang, Xiaojun and Bai, Hang and Duan, Yuhua and Yang, Bin and Leng, Li},
abstractNote = {Here, the impact of Pb in the tunnels of manganese oxide octahedral molecular sieves on chemical state of Mn species and lattice oxygen were investigated utilizing density functional theory calculations. The results show that the Pb dopant in the tunnels of OMS-2 could reduce the average valence states of Mn. The lower energy required for bulk oxygen defects formation in Pb-OMS-2 validates the activation of lattice oxygen by inclusion of tunnel dopant. The inclusion of Pb promotes the catalytic oxidation activity of OMS-2 by reducing the energy required for the surface lattice oxygen migration during the Mars – van Krevelen oxidation process.},
doi = {10.1016/j.cplett.2018.02.023},
journal = {Chemical Physics Letters},
number = C,
volume = 695,
place = {United States},
year = {2018},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 2 works
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Figures / Tables:

Fig. 1. Fig. 1. : The constructed 1 × 1 × 2 OMS-2 bulk and the (1 1 0) Miller facet OMS-2 slab for calculation. The purple spheres stand for the Mn atoms in spin up states and the blue spheres for the Mn atoms in spin down states. Red spheres represent the O atoms. The green spheremore » in the center represents the location of Pb in Pb-OMS-2 model. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)« less

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