Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume -, Issue -, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.202301135
Keywords
CO2 hydrogenation; oxygen vacancy; synergistic effect; zeolite
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In this study, the oxygen vacancy density in reducible Cr2O3 was increased by sequential carbonization and oxidation treatments, leading to high methanol selectivity of 98.1% in the direct hydrogenation of CO2 into aromatics at high temperature. Furthermore, by combining with acidic zeolite H-ZSM-5, the multifunctional catalyst achieved high conversion and selectivity of 25.4% and 80.1% (without CO) in the conversion of CO2 into aromatics. The acid site property in H-ZSM-5, especially the Al species located at the intersection of straight and sinusoidal channels, played a crucial role in enhancing aromatics selectivity, which could be controlled by varying the hydrothermal synthesis conditions. This work provides a synergistic strategy for improving the synthesis performance of aromatics from CO2 hydrogenation.
Even though the direct hydrogenation of CO2 into aromatics has been realized via a methanol-mediated pathway and multifunctional catalyst, few works have been focused on the simultaneously rational design of each component in multifunctional catalyst to improve the performance. Also, the structure-function relationship between aromatics synthesis performance and the different catalytic components (reducible metal oxide and acidic zeolite) has been rarely investigated. Herein, we increase the oxygen vacancy (O-v) density in reducible Cr2O3 by sequential carbonization and oxidation (SCO) treatments of Cr-based metal-organic frameworks. Thanks to the enriched O-v, Cr2O3-based catalyst affords high methanol selectivity of 98.1 % (without CO) at a CO2 conversion of 16.8 % under high reaction temperature (350 degrees C). Furthermore, after combining with the acidic zeolite H-ZSM-5, the multifunctional catalyst realizes the direct conversion of CO2 into aromatics with conversion and selectivity as high as 25.4 % and 80.1 % (without CO), respectively. The property of acid site in H-ZSM-5, especially the Al species that located at the intersection of straight and sinusoidal channels, plays a vital role in enhancing the aromatics selectivity, which can be precisely controlled by varying the hydrothermal synthesis conditions. Our work provides a synergistic strategy to boost the aromatics synthesis performance from CO2 hydrogenation.
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