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Study on carbon deposition associated with catalytic CH_4 reforming by using density functional theory

机译:密度泛函理论研究CH_4催化重整过程中的碳沉积

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摘要

Density functional theory (DFT) has been applied to investigate the adsorptions of CH_4, CH_3, CH_2, CH, C, H and dissociations CH_4, CH_3, CH_2, CH on the (111) catalyst surfaces of elementary metals Co bimetals NiFe. More important, the adsorptions and dissociations of those adspecies on elementary metals (Fe, Co, Ni and Cu) and bimetals (NiFe, NiCo and NiCu) have been analyzed. The adsorption energies, activation energies, reaction energies and d-band centers of the catalysts were calculated and their linear correlations were established. The adsorption energy decreases with the d-band center of the catalyst surface shift away from the Fermi level, and thus the increase in activation energy and reaction energy. Therefore, a good catalyst should have a moderate d-band center in CH_4/CO_2 reforming. This research finds that segregated NiCu is the best one among the eight CH_4/CO_2 reforming catalysts, Fe, Co, Ni, Cu, NiFe, NiCo, NiCu, and NiCu(S) [segregated NiCu].
机译:应用密度泛函理论(DFT)研究了CH_4,CH_3,CH_2,CH,C,H的吸附以及离解CH_4,CH_3,CH_2,CH在元素金属Co双金属NiFe的(111)催化剂表面上的吸附。更重要的是,已经分析了这些形态在元素金属(Fe,Co,Ni和Cu)和双金属(NiFe,NiCo和NiCu)上的吸附和解离。计算了催化剂的吸附能,活化能,反应能和d带中心,并建立了它们的线性关系。随着催化剂表面的d-带中心偏离费米能级,吸附能降低,因此活化能和反应能增加。因此,好的催化剂在CH_4 / CO_2重整中应具有适度的d带中心。研究发现,在Ni,Fe,Co,Ni,Cu,NiFe,NiCo,NiCu和NiCu(S)这8种CH_4 / CO_2重整催化剂中,偏析NiCu是最好的催化剂之一。

著录项

  • 来源
    《Fuel》 |2013年第11期|712-718|共7页
  • 作者单位

    Department of Chemical and Petroleum Engineering, University of Wyoming, 1000 E University Ave., Laramie, WY 82071, USA College of Chemistry and Chemical Engineering, Shanxi Datong University, Datong, Shanxi 037009, China Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan, Shanxi 030024, China;

    Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan, Shanxi 030024, China;

    Department of Chemical and Petroleum Engineering, University of Wyoming, 1000 E University Ave., Laramie, WY 82071, USA;

    Theoretical Division, Los Alamos National Laboratory, Los Alamos, NM 87545, USA;

    Western Research Institute, Laramie, WY 82070, USA;

    Department of Chemical and Petroleum Engineering, University of Wyoming, 1000 E University Ave., Laramie, WY 82071, USA;

    Department of Chemical and Petroleum Engineering, University of Wyoming, 1000 E University Ave., Laramie, WY 82071, USA;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    Catalytic CH_4 reforming; Carbon deposition; Density functional theory;

    机译:催化CH_4重整;碳沉积;密度泛函理论;

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