Investigation into sulfur poisoning processes in Ni-based catalysts using quantum-chemical computations

J. H. Wang*, Ming-Chang Lin, M. Liu

*Corresponding author for this work

研究成果: Conference contribution同行評審

摘要

Sulfur poisoning in Ni-based catalysts, one of the most critical problems in solid oxide fuel cells (SOFC), has been extensively examined at the atomic level by density functional theory (DFT). In the reversible poisoning process with atomic sulfur adsorption, the poisoning mechanism has been studied by elucidating the potential energy surface (PES) of the interfacial reactions between the sulfur contaminants (such as H2S) and Ni surfaces. The computed low reaction barriers (< 0.45 eV) and high exothermicities (< -2.51 eV) of the processes indicate that H2S can easily react and poison Ni surfaces. In the irreversible poisoning process forming nickel sulfide, the intrinsic properties of the nickel sulfide have been studied by examining its vibrational frequencies and density of states (DOS). The frequency analysis is vital to the identification with in-situ vibrational spectroscopy during the poisoning processes. The DOS analysis will be applied to understand the degradation behaviors (decrease of catalytic activity) in the sulfur-contaminated Ni catalysts. Furthermore, with thermodynamic corrections, a new computed Ni-S phase diagram precisely predicts the boundaries of the reversible and irreversible poisoning behaviors; the result agrees well with experimental observations.

原文English
主出版物標題American Chemical Society - 235th National Meeting, Abstracts of Scientific Papers
出版狀態Published - 1 十二月 2008
事件235th National Meeting of the American Chemical Society, ACS 2008 - New Orleans, LA, United States
持續時間: 6 四月 200810 四月 2008

出版系列

名字ACS National Meeting Book of Abstracts
ISSN(列印)0065-7727

Conference

Conference235th National Meeting of the American Chemical Society, ACS 2008
國家United States
城市New Orleans, LA
期間6/04/0810/04/08

指紋 深入研究「Investigation into sulfur poisoning processes in Ni-based catalysts using quantum-chemical computations」主題。共同形成了獨特的指紋。

引用此