The Evaluation and Mechanism Study of Zerovalent Iron (Fe0) Catalysts Supported on Coke for NO Reduction by H2

零价铁 焦炭 还原(数学) 催化作用 机制(生物学) 化学 化学工程 冶金 材料科学 工程类 物理化学 数学 有机化学 吸附 哲学 认识论 几何学
作者
Huanran Wang,Zheng Zhang,Lulu Zhao,Xianchun Li
出处
期刊:Chemical Engineering Research & Design [Elsevier BV]
卷期号:189: 911-919
标识
DOI:10.1016/j.psep.2024.06.143
摘要

Coke supported highly dispersed zerovalent iron Fe0 catalysts were synthesized and their catalytic activity in the reduction of NO by H2 was investigated using a fixed-bed reactor. The effect of H2 concentration on dispersion of active component Fe0 and activity of catalyst during preparation was investigated and density functional theory (DFT) simulation was used to study the reaction mechanism and the reason for catalyst deactivation. The Fe0 catalyst has a strong catalytic ability to reduce NO with H2. The activity of catalyst initially increased and then decreased in the increase of hydrogen concentration during the preparation. The carrier coke is not consumed in the reaction, which improves the dispersion of the active component Fe0. However, Fe0 catalyst is oxidized in the NO reduction, resulting in a decrease in the catalyst activity. The DFT calculations results suggest that the NO reduction follows the E-R mechanism, and the presence of Fe0 makes the N-O bond easily break to form N2. H2 has the capability to reduce oxidized Fe0 and release the catalytic active site, but the energy barrier that needs to be overcome is greater than that of oxidation of Fe0, which eventually leads to catalyst deactivation.
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