Coke relocation and Mo immobilization in donut-shaped Mo/HZSM-5 catalysts for methane dehydroaromatization
文献信息
Ming Cheng, Hugo Cruchade, Ludovic Pinard, Eddy Dib, Honghai Liu, Jiujiang Wang, Xinmei Liu, Zi-Feng Yan, Zhengxing Qin, Svetlana Mintova
Molybdenum-modified HZSM-5 catalysts are widely used for methane dehydroaromatization (MDA) but suffer from rapid deactivation due to coke formation. The limited diffusion in zeolitic catalysts promotes coke accumulation in micropores, creating concentration gradients of reactants and products within the crystals. In this study, we propose a synthesis approach to evaluate the impact of removing the crystal core in the Mo/HZSM-5 catalyst on the MDA performance. To achieve this, a parent zeolite (ZP) comprising a silicalite-1 core encased by an HZSM-5 crystal is subjected to two distinct treatments: fluorine (ZF) and alkaline (ZOH). These treatments dissolve the silicon-rich core, creating a central macropore in the crystals leading to the formation of donut-shaped catalysts. The alkaline treatment further generates additional mesopores and silanols by leaching atoms from the zeolite framework. The MDA reaction on molybdenum-impregnated zeolite catalysts (ZP, ZF, and ZOH) at 973 K was carried out. Interestingly, the “donut”-shaped catalysts modify the nature of the coke deposition, relocating the coke from the micropores to the macropores. Consequently, the removal of the crystal core effectively mitigates catalyst deactivation caused by coke formation. Moreover, the alkaline-treated catalyst exhibits additional beneficial properties, such as increased silanols and a higher surface area, which help to limit the sintering of molybdenum carbides during the MDA reaction. The new strategy improves the performance and stability of Mo/HZSM-5 catalysts in methane dehydroaromatization.
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Journal of Materials Chemistry A

Journal of Materials Chemistry A, B & C cover high quality studies across all fields of materials chemistry. The journals focus on those theoretical or experimental studies that report new understanding, applications, properties and synthesis of materials. The journals have a strong history of publishing quality reports of interest to interdisciplinary communities and providing an efficient and rigorous service through peer review and publication. The journals are led by an international team of Editors-in-Chief and Associate Editors who are all active researchers in their fields. Journal of Materials Chemistry A, B & C are separated by the intended application of the material studied. Broadly, applications in energy and sustainability are of interest to Journal of Materials Chemistry A, applications in biology and medicine are of interest to Journal of Materials Chemistry B, and applications in optical, magnetic and electronic devices are of interest to Journal of Materials Chemistry C. More than one Journal of Materials Chemistry journal may be suitable for certain fields and researchers are encouraged to submit their paper to the journal that they feel best fits for their particular article. Example topic areas within the scope of Journal of Materials Chemistry A are listed below. This list is neither exhaustive nor exclusive. Artificial photosynthesis Batteries Carbon dioxide conversion Catalysis Fuel cells Gas capture/separation/storage Green/sustainable materials Hydrogen generation Hydrogen storage Photocatalysis Photovoltaics Self-cleaning materials Self-healing materials Sensors Supercapacitors Thermoelectrics Water splitting Water treatment













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