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Role of formaldehyde in promoting aromatic selectivity during methanol conversion over gallium-modified zeolites

Gallium-modified HZSM-5 zeolites are known to increase aromatic selectivity in methanol conversion. However, there are still disputes about the exact active sites and the aromatic formation mechanisms over Ga-modified zeolites. In this work, in situ synchrotron radiation photoionization mass spectro...

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Detalles Bibliográficos
Autores principales: Wen, Wu, Xiao, Tianci, Feng, Beibei, Zhou, Chaoqun, Li, Jian, Ma, Hao, Zhou, Zhongyue, Zhang, Ying, Yang, Jiuzhong, Wang, Zhandong, Qi, Fei, Bao, Jun, Liu, Chengyuan, Pan, Yang
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9814038/
https://www.ncbi.nlm.nih.gov/pubmed/36697679
http://dx.doi.org/10.1038/s42004-022-00771-8
Descripción
Sumario:Gallium-modified HZSM-5 zeolites are known to increase aromatic selectivity in methanol conversion. However, there are still disputes about the exact active sites and the aromatic formation mechanisms over Ga-modified zeolites. In this work, in situ synchrotron radiation photoionization mass spectrometry (SR-PIMS) experiments were carried out to study the behaviors of intermediates and products during methanol conversion over Ga-modified HZSM-5. The increased formaldehyde (HCHO) yield over Ga-modified HZSM-5 was found to play a key role in the increase in aromatic yields. More HCHO was deemed to be generated from the direct dehydrogenation of methanol, and Ga(2)O(3) in Ga-modified HZSM-5 was found to be the active phase. The larger increase in aromatic production over Ga-modified HZSM-5 after reduction‒oxidation treatment was found to be the result of redispersed Ga(2)O(3) with smaller size generating a larger amount of HCHO. This study provides some new insights into the internal driving force for promoting the production of aromatics over Ga-modified HZSM-5.