[논문]Catalytic Interplay of Ga, Pt, and Ce on the Alumina Surface Enabling High Activity, Selectivity, and Stability in Propane Dehydrogenation

Kwon, Han Chang; Park, Younghwan; Park, Jeong Young; Ryoo, Ryong; Shin, Hyeyoung; Choi, Minkee

doi:10.1021/acscatal.1c02553

[해외논문] Catalytic Interplay of Ga, Pt, and Ce on the Alumina Surface Enabling High Activity, Selectivity, and Stability in Propane Dehydrogenation

ACS catalysis, v.11, 2021년, pp.10767 - 10777

Kwon, Han Chang (Department of Chemical and Biomolecular Engineering (BK21 Four) , Korea Advanced Institute of Science and Technology (KAIST) , Daejeon 34141 , Republic of Korea) , Park, Younghwan (Department of Chemical and Biomolecular Engineering (BK21 Four) , Korea Advanced Institute of Science and Technology (KAIST) , Daejeon 34141 , Republic of Korea) , Park, Jeong Young (Department of Chemistry , Korea Advanced Institute of Science and Technology (KAIST) , Daejeon 34141 , Republic of Korea) , Ryoo, Ryong (Department of Chemistry , Korea Advanced Institute of Science and Technology (KAIST) , Daejeon 34141 , Republic of Korea) , Shin, Hyeyoung , Choi, Minkee

Abstract ▼ AI-Helper

Pt-based bimetallic catalysts have been widely investigated in propane dehydrogenation (PDH) owing to their high activity in C-H cleavage and propylene selectivity. However, upon repeated coke oxidation for catalyst regeneration, they suffer from significant metal sintering and dealloying. Recently, γ-Al2O3 doped with Ga, Pt, and Ce was reported to exhibit superior catalytic activity, selectivity, and stability in PDH, but the catalytic role of each element has not been clearly understood because of the complexity of this system. In this study, we rigorously investigated the reaction mechanism and catalytic interplay of each component (Ga, Pt, and Ce). Selective poisoning, in situ diffuse reflectance infrared Fourier transform spectroscopy, and H2-D2 exchange revealed that Ga3+ is responsible for the heterolytic dissociation of the C-H bond of propane, while Pt0 facilitates the sluggish H recombination into H2 via reverse spillover. Catalyst deactivation during repeated reaction-regeneration cycles is mainly due to the irreversible sintering of Pt0. Notably, optimal Ce doping (∼2 wt %) selectively generated atomically dispersed Ce3+ sites on the γ-Al2O3 surface, which greatly suppressed the sintering of Pt0 particles by increasing the metal-support interactions. In contrast, excessive Ce loading generated discrete CeO2 domains, which stabilized the Pt species in the form of Pt2+ inactive for H recombination. Thus, excessive Ce loading led to an even more severe loss of catalytic activity and selectivity. The present results demonstrate that the selective generation of atomically dispersed Ce3+ on the γ-Al2O3 surface is important for stabilizing Pt0 species, which is essential for simultaneously achieving high catalytic activity, selectivity, and longevity in PDH.[FIG OMISSION]

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