期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 127, 期 13, 页码 6356-6370出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.3c01306
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The direct conversion of carbon dioxide into aromatic compounds provides an environmentally friendly resource for aromatic chemicals with high global demand. Bifunctional catalysts composed of ZnZrOx and ZSM-5 showed improved aromatics yields by decreasing the ZSM-5 domain size. However, for a physical mixture of catalyst components, the particle size of ZnZrOx increased due to the inverse impact of ZSM-5 crystal size, resulting in enhanced diffusion barriers for small crystals of ZSM-5. Larger crystals of ZSM-5 can be used to obtain a higher concentration of benzene, toluene, and xylene.
The direct conversion of carbon dioxide into aromatic compounds may provide an environmentally friendly resource for a family of chemical building blocks wit h high global demand-aromatic chemicals. An array of bifunctional catalysts composed of ZnZrOx for the conversion of CO2 to methanol and ZSM-5 for methanol aromatization is evaluated considering multiple operational and catalytic parameters, with a focus on the particle size of each catalyst functionality. Aromatic yields generally increase as the ZSM-5 domain size decreases for different configurations of catalyst domains-mixed powders, mixed pellets, and separate beds. However, for a physical mixture of the catalyst components prior to pelletization (mixed powder case), varying the ZSM-5 crystal size inversely impacts the particle size of ZnZrOx, leading to enlarged metal oxide domains and enhanced intermediate diffusion barriers for very small crystals of ZSM-5. Larger crystals of ZSM-5 can be employed to obtain a higher concentration of benzene, toluene, and xylene (BTX) among aromatics. Upon employing a physical mixture of the ZnZrOx/ZSM-5 catalyst with a Si/Al ratio of 300 and a ZSM-5 crystal size of 300 nm, a total aromatics selectivity of 44% at CO2 conversion of 6% was obtained at 320 degrees C, WHSV of 7200 mL gcatalyst-1 h-1, and H2/CO2 ratio of 3.
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