3D-printed zeolite monoliths with hierarchical porosity for selective methanol to light olefin reaction
文献情報
Xin Li, Fateme Rezaei, Ali A. Rownaghi
Herein, we report the rapid synthesis of customized zeolite monoliths with various compositions and hierarchical porosity (macro–meso–micro) using a 3D printing technique. Moreover, several 3D-printed monoliths were synthesized from HZSM-5 and HZSM-5/silica, and SAPO-34 crystals were grown on the as-synthesized 3D-printed ZSM-5 monoliths via a secondary growth method. The 3D-printed zeolite monoliths exhibited hierarchical porosity with pore sizes ranging from 1.5 nm to 1 μm. Characterization results suggested that transformation of zeolite paste into the monolith structure enhanced the mesopore volume and moderated the acidity of the structures. Further incorporation of amorphous silica into the HZSM-5 monoliths reduced the acid site density. The obtained monoliths were evaluated in the methanol to olefin (MTO) reaction and found to exhibit higher stability than their powder counterparts. The selectivity to light olefins was significantly increased as a result of modification in the acidity and porosity of the monolith catalysts, which in turn mitigated the hydrogen transfer, hence suppressing the formation of paraffins and aromatics. The SAPO-34 coating tended to increase the ethylene selectivity due to its intrinsic framework structure. The analysis of spent zeolite monoliths by TGA-DTA indicated that the amount of polyaromatic species formed during the reaction was much lower than that on the powder analogues, due to their diluted acid site density and decreased Brønsted acid sites, as proven by NH3-TPD profiles and py-FTIR spectra. Furthermore, 29Si MAS NMR results confirmed slight dealumination of 3D-printed monoliths after the MTO reaction.
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Reaction Chemistry & Engineering

Reaction Chemistry & Engineering is an interdisciplinary journal reporting cutting-edge research focused on enhancing the understanding and efficiency of reactions. Reaction engineering leverages the interface where fundamental molecular chemistry meets chemical engineering and technology. Challenges in chemistry can be overcome by the application of new technologies, while engineers may find improved solutions for process development from the latest developments in reaction chemistry. Reaction Chemistry & Engineering is a unique forum for researchers whose interests span the broad areas of chemical engineering and chemical sciences to come together in solving problems of importance to wider society. All papers should be written to be approachable by readers across the engineering and chemical sciences. Papers that consider multiple scales, from the laboratory up to and including plant scale, are particularly encouraged.




