Controlling N2O formation during regeneration of NOx storage and reduction catalysts: from impact of platinum-group metal type to rational utilization

Literature Information

Publication Date 2017-11-15
DOI 10.1039/C7CP05659A
Impact Factor 3.676
Authors

Jinxin Zhu, Jun Wang, Jianqiang Wang, Mingxin Dong


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Abstract

Herein, we report an effective strategy for minimization of N2O emissions based on elucidating the impact of the type of platinum-group metals (PGMs = Pt, Pd, or Rh) on by-product formation during regeneration of PGM–BaO/Al2O3 catalysts. The significant differences in N2O or NH3 formation were thoroughly investigated from the perspective of an in situ reaction. Kinetic analysis of NO reduction by CO shows different turnover frequency and apparent activation energy values over these catalysts. The results reveal that the apparent kinetics is dependent on the type of platinum-group metal chosen. In situ DRIFTS data indicate that the unique adsorption behaviors of reactants via which they access each PGM essentially determine their individual reaction kinetics. The preferential adsorption of NO or CO molecules on the PGM surface controls the dominant intermediate (NOad/Nad, COad, or NCOad) species, which is a major factor responsible for various yields of N2O and NH3 during the rich period. Finally, a feasible strategy has been proposed via optimizing catalyst formulation to effectively control the N2O emissions.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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