Catalytic Activity of Tandem Catalysts Based on ZnGa2O4 and MFI Zeolite in CO2 Hydrogenation

IF 1.3 4区工程技术 Q3 CHEMISTRY, ORGANIC

Petroleum Chemistry Pub Date : 2024-10-30 DOI:10.1134/S0965544124060070

G. K. Ivanov, A. A. Maerle, D. O. Bachurina, I. V. Dobryakova, I. I. Ivanova

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Abstract

A series of tandem catalysts based on a ZnGa₂O₄ spinel and on MFI-type acidic components with varying SiO₂/Al₂O₃ ratios were prepared by mechanical mixing at a spinel to MFI weight ratio of 2 : 1. These catalysts were tested in the conversion of carbon dioxide to olefins at 380°C and 27 bar. The hydrogenating component (ZnGa₂O₄) was prepared by co-precipitation of the corresponding hydroxides followed by heat treatment. The zeolites were synthesized by steam-assisted crystallization. A reference catalyst was prepared from ZnGa₂O₄ and a hydrothermally synthesized commercial zeolite CBV28014. The physicochemical properties of the catalysts and their components were characterized by low-temperature nitrogen adsorption–desorption, chemical analysis, NH₃-TPD, H₂-TPR, XRD, and SEM. The sample with the highest SiO₂/Al₂O₃ ratio (250) achieved the highest CO₂ conversion; this parameter dropped as the aluminum content in the samples increased. The highest selectivity towards light olefins was observed for the catalyst with SiO₂/Al₂O₃ = 172 in the acidic component, likely because this zeolite had an optimum acidity for the production of light olefins.

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ZnGa2O4 - MFI分子筛串联催化剂在CO2加氢中的催化活性

以ZnGa2O4尖晶石和不同SiO2/Al2O3比的MFI型酸性组分为原料，在尖晶石与MFI重量比为2:1的条件下，通过机械混合制备了一系列串联催化剂。在380℃、27 bar的条件下对这些催化剂进行了二氧化碳制烯烃的实验。加氢组分ZnGa2O4是通过氢氧化物共沉淀法和热处理制备的。采用蒸汽辅助结晶法合成沸石。以ZnGa2O4和水热合成的商业沸石CBV28014为原料制备了参考催化剂。采用低温氮吸附-脱附、化学分析、NH3-TPD、H2-TPR、XRD、SEM等手段表征了催化剂及其组分的理化性质。SiO2/Al2O3比值最高（250）的样品CO2转化率最高；该参数随样品中铝含量的增加而下降。在酸性组分中，SiO2/Al2O3 = 172的分子筛对轻烯烃的选择性最高，这可能是因为该分子筛具有最佳的酸性来生产轻烯烃。

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来源期刊

Petroleum Chemistry 工程技术-工程：化工

CiteScore

2.50

自引率

21.40%

发文量

102

审稿时长

6-12 weeks

期刊介绍： Petroleum Chemistry (Neftekhimiya), founded in 1961, offers original papers on and reviews of theoretical and experimental studies concerned with current problems of petroleum chemistry and processing such as chemical composition of crude oils and natural gas liquids; petroleum refining (cracking, hydrocracking, and catalytic reforming); catalysts for petrochemical processes (hydrogenation, isomerization, oxidation, hydroformylation, etc.); activation and catalytic transformation of hydrocarbons and other components of petroleum, natural gas, and other complex organic mixtures; new petrochemicals including lubricants and additives; environmental problems; and information on scientific meetings relevant to these areas. Petroleum Chemistry publishes articles on these topics from members of the scientific community of the former Soviet Union.