Role of surface frustrated Lewis pairs on reduced CeO2(110) in direct conversion of syngas

doi:10.1016/S1872-2067(20)63627-0

Abstract

Abstract: Direct syngas conversion to light olefins on bifunctional oxide-zeolite (OX-ZEO) catalysts is of great interest to both academia and industry, but the role of oxygen vacancy (Vo) in metal oxides and whether the key intermediate in the reaction mechanism is ketene or methanol are still not well-understood. To address these two issues, we carry out a theoretical study of the syngas conversion on the typical reducible metal oxide, CeO₂, using density functional theory calculations. Our results demonstrate that by forming frustrated Lewis pairs (FLPs), the V_Os in CeO₂ play a key role in the activation of H₂ and CO. The activation of H₂ on FLPs undergoes a heterolytic dissociative pathway with a tiny barrier of 0.01 eV, while CO is activated on FLPs by combining with the basic site (O atom) of FLPs to form CO₂^2-. Four pathways for the conversion of syngas were explored on FLPs, two of which are prone to form ketene and the other two are inclined to produce methanol suggesting a compromise to resolve the debate about the key intermediates (ketene or methanol) in the experiments. Rate constant calculations showed that the route initiating with the coupling of two CO* into OCCO* and ending with the formation of ketene is the dominant pathway, with the neighboring FLPs playing an important role in this pathway. Overall, our study reveals the function of the surface FLPs in the activation of H₂ and CO and the reaction mechanism for the production of ketene and methanol for the first time, providing novel insights into syngas conversion over OX-ZEO catalysts.

Key words: Syngas conversion, Light olefins, Oxide-zeolite, Frustrated Lewis pairs, CeO₂

Zheng-Qing Huang, Teng-Hao Li, Bolun Yang, Chun-Ran Chang. Role of surface frustrated Lewis pairs on reduced CeO₂(110) in direct conversion of syngas[J]. Chinese Journal of Catalysis, 2020, 41(12): 1906-1915.

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Role of surface frustrated Lewis pairs on reduced CeO₂(110) in direct conversion of syngas

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