Quantifying the impact of dispersion, acidity and porosity of Mo/HZSM-5 on the performance in methane dehydroaromatization

The catalytic performance of the bifunctional catalyst Mo/HZSM-5 for methane dehydroaromatization (MDA) depends on the Mo dispersion and on zeolite acidity. Here we separately quantify the effect of dispersion and the effect of acidity on aromatic yields and coke selectivity. Also, the effect of porosity on the same is quantitatively...

A site-sensitive quasi-in situ strategy to characterize Mo/HZSM-5 during activation

The active sites on the methane dehydroaromatization (MDA) catalyst Mo/HZSM-5 are very hard to characterize, because they are present in various geometries and sizes and only form under reaction conditions with methane at 700 °C. To address these issues an experimental strategy is presented that enables distinguishing different active sites...

Revealing Lattice Expansion of Small-Pore Zeolite Catalysts during the Methanol-to-Olefins Process Using Combined Operando X-ray Diffraction and UV-vis Spectroscopy

In small-pore zeolite catalysts, where the size of the pores is limited by eight-ring windows, aromatic hydrocarbon pool molecules that are formed inside the zeolite during the Methanol-to-Olefins (MTO) process cannot exit the pores and are retained inside the catalyst. Hydrocarbon species whose size is comparable to the size of the zeolite...

Progress in Developing a Structure-Activity Relationship for the Direct Aromatization of Methane

To secure future supply of aromatics, methane is a commercially interesting alternative feedstock. Direct conversion of methane into aromatics combines the challenge of activating one of the strongest C-H bonds in all hydrocarbons with the selective aromatization over zeolites. To address these challenges, smart catalyst and process design...

Facile manufacture of porous organic framework membranes for precombustion CO₂ capture

The development of new membranes with high H₂ separation performance under industrially relevant conditions (high temperatures and pressures) is of primary importance. For instance, these membranes may facilitate the implementation of energy-efficient precombustion CO₂ capture or reduce energy intensity in other...

On the dynamic nature of Mo sites for methane dehydroaromatization

The mechanism of methane activation on Mo/HZSM-5 is not yet fully understood, despite the great interest in methane dehydroaromatization (MDA) to replace aromatics production in oil refineries. It is difficult to assess the exact nature of the active site due to fast coking. By pre-carburizing Mo/HZSM-5 with carbon monoxide (CO), the MDA active...

Benzimidazole linked polymers (BILPs) in mixed-matrix membranes: Influence of filler porosity on the CO₂/N₂ separation performance

The performance of mixed-matrix membranes (MMMs) based on Matrimid^® and benzimidazole-linked polymers (BILPs) have been investigated for the separation CO₂/N₂ and the dependency on the filler porosity. BILPs with two different porosities (BILP-101 and RT-BILP-101) were synthesized through controlling the...

Relevance of the Mo-precursor state in H-ZSM-5 for methane dehydroaromatization

Although the local geometry of Mo in Mo/HZSM-5 has been characterized before, we present a systematic way to manipulate the configuration of Mo and link it to its catalytic properties. The location and geometry of cationic Mo-complexes, the precursor of the active metal site for methane dehydroaromatization, are altered by directing the way...

Insights into the Activity and Deactivation of the Methanol-to-Olefins Process over Different Small-Pore Zeolites As Studied with Operando UV-vis Spectroscopy

The nature and evolution of the hydrocarbon pool (HP) species during the Methanol-to-Olefins (MTO) process for three small-pore zeolite catalysts, with a different framework consisting of large cages interconnected by small eight-ring windows (CHA, DDR, and LEV) was studied at reaction temperatures between 350 and 450 °C using a combination...

Engineering Selective and Stable Methanol to Olefins Catalysts

Consequences of secondary zeolite growth on catalytic performance in DMTO studied over DDR and CHA

Zeolites with DDR (Sigma-1 and ZSM-58) and CHA (SSZ-13) topology were synthesized by seed assisted and direct hydrothermal synthesis in order to investigate the effects of fast crystal growth on catalytic performance. Application of small amount of seeds (0.1% wt) significantly reduced synthesis time of all the studied zeolites. XRD and NH...

The importance of heat effects in the Methanol to Hydrocarbons reaction over ZSM-5: on the role of mesoporosity on catalyst performance

Interpretation of catalytic performance during the MTH process is hampered by heat transport phenomena. We demonstrate that large temperature rises can occur during fixed bed labscale catalyst testing of ZSM-5, even when a large catalyst bed dilution is applied. Formation of mesopores in ZSM-5 leads to partial mitigation of these effects because...

Methanol-to-olefins process over zeolite catalysts with DDR topology: Effect of composition and structural defects on catalytic performance

A systematic study of the effect of physicochemical properties affecting catalyst deactivation, overall olefin selectivity and ethylene/propylene ratio during the methanol-to-olefins (MTO) reaction is presented for two zeolites with the DDR topology, namely Sigma-1 and ZSM-58. Both catalysts show high selectivity towards light olefins and...

Methanol-to-olefins process over zeolite catalysts with DDR topology: Effect of composition and structural defects on catalytic performance

A systematic study of the effect of physicochemical properties affecting catalyst deactivation, overall olefin selectivity and ethylene/propylene ratio during the methanol-to-olefins (MTO) reaction is presented for two zeolites with the DDR topology, namely Sigma-1 and ZSM-58. Both catalysts show high selectivity towards light olefins and...