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N2O Formation Mechanism and Suppression Strategy on Pt Catalysts for NO x Removal from Hydrogen-Internal Combustion
Shaohua Xie1, Yuejin Li2, Kailong Ye1
1Department of Chemical and Environmental Engineering, Bourns College of Engineering, Center for Environmental Research and Technology (CE-CERT), Materials Science and Engineering (MSE) Program, UCR Center for Catalysis, University of California, Riverside, California 92521, United States.
Abstract:
Pt-based catalysts exhibit excellent low-temperature activity in the selective catalytic reduction of NO x with H2 (H2-SCR), but their tendency to form N2O poses a significant challenge for practical use. This issue is further complicated by unclear formation mechanisms, hindering the development of more efficient catalysts. This study explored the N2O generation mechanisms on Pt catalysts supported by MgO, Al2O3, SiO2, and TiO2, aiming to achieve a deep understanding that could advance the Pt catalysts with high NO x conversion and minimized N2O emissions. Through systematic kinetics and characterization analyses, the direct influence of the support acidity and reactant dynamics (O2 and NO) on N2O formation was clearly revealed. Notably, the Pt catalysts with strong NO adsorption capacity showed reduced N2O generation, highlighting the critical role of NO adsorption sites in the H2-SCR process. By incorporation of NO adsorption sites (i.e., MgO, BaO, CeO2) onto Pt/SiO2, both the H2-SCR efficiency and N2 selectivity (reduced N2O selectivity) were significantly enhanced, effectively reducing the N2O emissions through optimized surface NO adsorption. These findings provide a design framework for more selective Pt-based catalysts, advancing H2-SCR systems for effective NO x abatement from hydrogen-internal combustion engines, which is a promising carbon-free transportation technology.
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