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Development of a New Ternary Al₂O₃-HAP-Pd Catalyst for Diethyl Ether and Ethylene Production Using the Preferential Dehydration of Ethanol.

ABSTRACT: This study aims to convert ethanol to higher value-added products, particularly diethyl ether and ethylene using the catalytic dehydration of ethanol. Hence, the gas-phase dehydration of ethanol over Al₂O₃-HAP catalysts as such and modified by addition of palladium (Pd) in a microreactor was evaluated. The commercial Al₂O₃-HAP catalyst was first prepared by the physical mixing method, and then, the optimal ratio of the Al₂O₃-HAP catalyst (2:8 by wt %) was impregnated with Pd to develop a new functional catalyst to alter surface acidity. Based on the results, the combination of Al₂O₃ and HAP catalysts generated significant quantities of weak acid sites which demonstrates an enhancement in catalytic activity. In addition, Pd modification in the optimal composition ratio of the Al₂O₃-HAP catalyst extremely increased the amount of weak acid sites as well as weak acid density due to the synergistic effect between the Pd and Al₂O₃-HAP catalyst that are supposed to suggest the active sites in the reaction. Among all catalysts, the Al20-HAP80-Pd catalyst displayed brilliant catalytic performance in the course of diethyl ether yield (ca. 51.0%) at a reaction temperature of 350 °C and ethylene yield (ca. 75.0%) at a reaction temperature of 400 °C having an outstanding stability under time-on-stream for 10 h. This is recognized to the combination of the effects of weak acid sites (Lewis acidity), small amount of strong acid sites, and structural characteristics of the catalytic materials used.

SUBMITTER: Autthanit C

PROVIDER: S-EPMC8340412 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Methanol synthesized from carbonate hydrogenation is of great importance for CO2 utilization indirectly. Herein, a series of Cu/Zn/Al heterogeneous catalysts were prepared by co-precipitation with a synchronous aging step, and were applied for hydrogenation of diethyl carbonate (DEC) to produce methanol. Furthermore, the catalysts were characterized by physicochemical methods, such as N2 adsorption, ICP-OES, N2O titration, SEM, TEM, XRD, H2-TPR and XPS in detail. Higher copper concentration led to a higher ratio of bulk CuOx species in the calcined samples, which resulted in different copper species distribution after the reduction process. Structure activity relationship analysis indicated that the balance of surface Cu0 and Cu+ species influenced the formation rate of methanol. A higher proportion of Cu+ to (Cu+ + Cu0) was conductive to methanol formation, while excessive Cu0 site density played a negative influence on the methanol synthesized from DEC. Cu/Zn/Al with a 45.2% weight fraction of copper showed better performance with a total methanol formation rate of 131.0 mg gcat. -1 h-1. The reaction temperature and reaction time could obviously affect the reaction performance and the results suggested that 200 °C and 6 h were suitable. Furthermore, the long-term stability and activity of the catalyst was also studied on a fixed bed, and the yield of total methanol reached to 88.5% and the selectivity of total methanol gradually decreased to 74.0% within 200 h, which could be attributed to the detrimental influence derived from the increase of Cu0. The reaction pathways involved in the hydrogenation of DEC process were proposed. The substance scope was also extended to other carbonates and the catalyst exhibited superior catalytic performance toward linear carbonates. This work provided insights into carbonate hydrogenation over an effective Cu/Zn/Al catalyst, which could be utilized into upgrading CO2 indirectly to produce commodity methanol under relatively mild reaction conditions.

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Development of a New Ternary Al₂O₃-HAP-Pd Catalyst for Diethyl Ether and Ethylene Production Using the Preferential Dehydration of Ethanol.

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Development of a New Ternary Al2O3-HAP-Pd Catalyst for Diethyl Ether and Ethylene Production Using the Preferential Dehydration of Ethanol.

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Development of a New Ternary Al₂O₃-HAP-Pd Catalyst for Diethyl Ether and Ethylene Production Using the Preferential Dehydration of Ethanol.