Support Induced Effects on the Ir Nanoparticles Activity, Selectivity and Stability Performance under CO(2) Reforming of Methane

载体对铱纳米粒子在甲烷CO₂重整反应中的活性、选择性和稳定性的影响

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Abstract

The production of syngas (H(2) and CO)-a key building block for the manufacture of liquid energy carriers, ammonia and hydrogen-through the dry (CO2-) reforming of methane (DRM) continues to gain attention in heterogeneous catalysis, renewable energy technologies and sustainable economy. Here we report on the effects of the metal oxide support (γ-Al(2)O(3), alumina-ceria-zirconia (ACZ) and ceria-zirconia (CZ)) on the low-temperature (ca. 500-750 ∘C) DRM activity, selectivity, resistance against carbon deposition and iridium nanoparticles sintering under oxidative thermal aging. A variety of characterization techniques were implemented to provide insight into the factors that determine iridium intrinsic DRM kinetics and stability, including metal-support interactions and physicochemical properties of materials. All Ir/γ-Al(2)O(3), Ir/ACZ and Ir/CZ catalysts have stable DRM performance with time-on-stream, although supports with high oxygen storage capacity (ACZ and CZ) promoted CO(2) conversion, yielding CO-enriched syngas. CZ-based supports endow Ir exceptional anti-sintering characteristics. The amount of carbon deposition was small in all catalysts, however decreasing as Ir/γ-Al(2)O(3) > Ir/ACZ > Ir/CZ. The experimental findings are consistent with a bifunctional reaction mechanism involving participation of oxygen vacancies on the support's surface in CO(2) activation and carbon removal, and overall suggest that CZ-supported Ir nanoparticles are promising catalysts for low-temperature dry reforming of methane (LT-DRM).

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