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Selective Light Hydrocarbon Production from CO2 Hydrogenation over Na/ZnFe2O4 and CHA-Zeolite Hybrid Catalysts

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Title
Selective Light Hydrocarbon Production from CO<sub>2</sub> Hydrogenation over Na/ZnFe<sub>2</sub>O<sub>4</sub> and CHA-Zeolite Hybrid Catalysts
Author(s)
Ra, Eun Cheol; Kim, Kwang Hyun; Lee, Ju Hyeong; Jang, Sejin; Kim, Hyo Eun; Lee, Jin Ho; Kim, Eun Hyup; Kim, Haneul; Ja Hun Kwak; Jae Sung Lee
Publication Date
2024-03
Journal
ACS Catalysis, v.14, no.5, pp.3492 - 3503
Publisher
American Chemical Society
Abstract
Carbon dioxide hydrogenation to value-added fuels and chemicals has been studied widely as a means to recycle the most-troublesome greenhouse gas. The reaction produces hundreds of different chemicals, and therefore, selectivity control toward specific desired products is of paramount importance. In this study, a hybrid catalyst system consisting of Na/ZnFe2O4 (ZFO) and a CHA-zeolite (SSZ-13 or SAPO-34) is developed to maximize C-2-C-4 light hydrocarbon production. Utilizing the compact 3.8 & Aring; pore size of CHA-zeolites, the Na/ZnFe2O4 catalyst-produced long-chain hydrocarbons are efficiently shortened to C-2-C-4 hydrocarbons with over 55% selectivity in the hybrid systems. Notably, ZFO + SAPO-34 shows a preference for light olefins, while ZFO + SSZ-13 uniquely enhances selectivity for C-3 products. The difference is attributed to the much stronger acid sites present in SSZ-13 than in SAPO-34, which promote hydrogenation of olefins and the ethylene-to-propane conversion reaction in particular. Further modification of SSZ-13 with steam treatment leads to the dealumination of its framework and an enhanced activity of the ethylene-to-propane reaction, yielding 32.8% of C-3-selectivity. Accordingly, a hybrid catalytic system combining a CO2 Fischer-Tropsch catalyst with a CHA-zeolite is a promising route to produce light hydrocarbons from CO2 hydrogenation more selectively than single catalysts. This work also demonstrates that acidity control could be a powerful tool to manipulate the reaction pathway that occurs on zeolite catalysts.
URI
https://pr.ibs.re.kr/handle/8788114/14904
DOI
10.1021/acscatal.4c00099
ISSN
2155-5435
Appears in Collections:
Center for Multidimensional Carbon Materials(다차원 탄소재료 연구단) > 1. Journal Papers (저널논문)
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