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In the present study, we prepared a 12 nm thick Ir overlayer via pulsed cathodic arc plasma deposition on a 50 μm thick Fe-Cr-Al metal (SUS) foil. Using this thin-film catalyst made NH 3 -O 2 reactions more environmentally benign due to a much lower selectivity for undesirable N 2 O (<5%) than that of a Pt overlayer (∼70%) at 225 °C. Despite its small surface area, Ir/SUS exhibited promising activity as an ammonia slip catalyst according to a turnover frequency (TOF) >70-fold greater than that observed with conventional Ir nanoparticle catalysts supported on γ-Al 2 O 3 . We found that the high-TOF NH 3 oxidation was associated with the stability of the metallic Ir surface against oxidation by excess O 2 present in simulated diesel exhaust. Additionally, we found that the Ir overlayer structure was thermally unstable at reaction temperatures ≥400 °C and at which point the Ir surface coverage dropped significantly; however, thermal deterioration was substantially mitigated by inserting a 250 nm thick Zr buffer layer between the Ir overlayer and the SUS foil substrate (Ir/Zr/SUS). Although N 2 O formation was suppressed by NH 3 oxidation over Ir/Zr/SUS, other undesired byproducts (i.e., NO and NO 2 ) were readily converted to N 2 by coupling with a V 2 O 5 -WO 3 /TiO 2 catalyst in a second reactor for selective catalytic reduction by NH 3 . These results demonstrated that this tandem reactor configuration converted NH 3 to N 2 with nearly complete selectivity at a range of 200-600 °C in the presence of excess O 2 (8%) and H 2 O (10%)., Competing Interests: The authors declare no competing financial interest., (© 2020 The Authors. Published by American Chemical Society.)