Structural Properties of PtCuO/Al2O3 surface catalyst for selective NH3 oxidation using operando spectroscopy

01 December 2023, Version 1

Abstract

Selective catalytic oxidation (SCO) of NH3 to N2 is one of the most effective methods to eliminate NH3 emissions. However, achieving high conversion over a wide operating temperature range while avoiding over-oxidation to NOx is a significant challenge. Commercial Pt catalysts have full NH3 conversion at low temperatures but suffer from low N2 selectivity. To mitigate this challenge, it is crucial to limit the over-oxidation of NH3. In this study, we developed a bi-metal surface catalyst with improved Pt atom efficiency. The PtSCuO/Al2O3 catalyst consists of Pt atoms on the surface of CuO nanoparticles. It achieves full NH3 conversion at 250 °C with WHSV of 600 mlNH3h-1g-1 which is 50 °C lower than the commercial Pt/Al2O3, and maintains high N2 selectivity through all temperature window (150-450 °C). At 200 °C, PtSCuO/Al2O3, exhibited a staggering 30-fold increase in activity compared to the commercial Pt/Al2O3. Operando XAFS studies reveal that the surface Pt atoms in PtSCuO/Al2O3 not only enhance the redox ability of Cu species but also alter the redox rate of Cu species, which improves the while reaction rate of the NH3-SCO reaction. Moreover, the synergistic effect of Pt sites and Cu sites in PtSCuO/Al2O3 contributes to improved selectivity via the internal selective catalytic reduction (i-SCR) route.

Keywords

bimetallic catalyst
Selective catalytic oxidation
QXAFS

Supplementary materials

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SUpplementary information
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methods, figures and tables
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