Durability improvements of H-ZSM-5 zeolite for ethanol conversion after treatment with chelating agents

Däumer, Daniel; Seifert, Markus; Reschetilowski, Wladimir

doi:10.1016/j.micromeso.2015.07.031

Cited by 12 publications

(13 citation statements)

References 38 publications

(51 reference statements)

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“…[21,24] In most cases the dealumination of zeolites in the liquid phase, e. g. by use of mineral acids leads to non-negligible structural damages. [11] Gas phase dealumination as in the case of hydrothermal treatment or by use of volatile SiCl 4 improves efficiency of dealumination processes.…”

Section: Exemplary Methods For Framework Dealuminationmentioning

confidence: 99%

“…[10] Initially little influence of EFSPE (extra-framework species) on ethanol conversion in H-ZSM-5 is detected by use of chelating agents avoiding overabundant dealumination of the zeolite framework. [11] The main goal of this work is to improve the short-term durability of commercial H-ZSM-5 zeolite during the conversion of ethanol to aromatics by a targeted framework dealumination. Based on the assessment of positive and negative effects of each post-synthetic procedure, a combination of treatment methods is proposed and tested.…”

Section: Introductionmentioning

confidence: 99%

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Ethanol to Aromatics on Modified H‐ZSM‐5 Part I: Interdependent Dealumination Actions

et al. 2020

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In this study a H‐ZSM‐5 zeolite (Si/Al=11) was modified by a stepwise treatment with steam, sodium hydroxide and hydrochloric acid. During progressing dealumination by various treatment methods, the drawbacks of initial post‐synthetic steps, e. g. pore‐filling by steam dealumination, are compensated by subsequent steps, e. g. washing by acid, which leads to a scientifically based preparation of required ZSM‐5 zeolite. Solid‐state properties of as‐synthesized and modified zeolites are determined by structural (XRD, ICP‐OES, NMR), textural (physisorption, laser scattering) and acid sites analysis (TPAD). Consequently, extended dealumination without structural damage is demonstrated. Its origin by framework dealumination and pore cleaning is verified in ethanol to hydrocarbon process (ETH) by shape‐selective formation of coke and aromatics, characterized by “aromatics index” (AI).

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Section: Exemplary Methods For Framework Dealuminationmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Ethanol to Aromatics on Modified H‐ZSM‐5 Part I: Interdependent Dealumination Actions

et al. 2020

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“…Previous investigations revealed scientifically based combinations of dealumination methods to reduce acid site density, to clean pore channels from residual extra-framework species (EFSPE) and to enhance aromatics yields. [9,10] The main goal of this work now is to study short-term durability behavior of H-ZSM-5 zeolites during conversion of ethanol to aromatics by variation of inert gas flow and contact time, respectively. Based on a commercial and modified H-ZSM-5 zeolite durability and selectivity trends with varying inert gas flow reveal unexpected distinct product formation parameters for aromatics and coke formation and a decoupling of catalyst decay from coking.…”

Section: Scope Of This Workmentioning

confidence: 99%

Ethanol to Aromatics on Modified H‐ZSM‐5 Part II: An Unexpected Low Coking

Seifert

Marschall

Gille

et al. 2020

Chemistry An Asian Journal

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In this study a commercial H-ZSM-5 zeolite (Si/Al = 11) was post-synthetically modified by a combined dealumination procedure to adjust its catalytic properties for the selective formation of aromatics from ethanol. The solid-state properties of original and modified zeolites are determined by structural, textural and acidity analysis. The formation of aromatics and durability of the zeolites were investigated depending on space velocity or contact time in the catalyst bed. In particular, the formation rate and desorption of aromatics from solid-state surface as well as their tendency to form coke precursors by consecutive build-up reactions determine the formation of coke. Therefore, the rate of buildup and finished aromatization by hydride transfer (predetermined by the kind, location and geometric arrangement of surface acid sites) and the statistical number of reaction events until final desorption at the specific contact time have to be harmonized to increase aromatics yield and to decrease catalyst decay by coke simultaneously.

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“…) in the presence of HAlBEA zeolite is initially formed, which probably results from the consecutive reactions of ethylene. Direct production of C2-C4 olefins and higher hydrocarbons (gasoline-range) by the conversion of bioethanol (ethanol to gasoline, ETG) has recently gained great interests [64][65][66][67][68]. Formation of propane can be directly related to the higher acidity of HAlBEA zeolite.…”

Section: Catalytic Performance In the Steam Reforming Of Ethanolmentioning

confidence: 99%

Effects of dealumination on the performance of Ni-containing BEA catalysts in bioethanol steam reforming

Gac

Greluk

Słowik

et al. 2018

Applied Catalysis B: Environmental

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The effects of dealumination of BEA zeolite on the formation of nickel active sites and the performance of Nicontaining BEA zeolite catalysts in the steam reforming of ethanol have been studied. Ni-containing BEA zeolite catalysts were prepared by the impregnation of unmodified and dealuminated BEA zeolites with Ni(NO 3) 2 precursor. The properties of Ni 10 HAlBEA and Ni 10 SiBEA zeolite catalysts were studied by means of X-ray diffraction, 1 H, 27 Al and 29 Si magic-angle spinning nuclear magnetic resonance, Fourier-transform infrared and Raman spectroscopy, transmission electron microscopy, temperature-programmed reduction, temperature-programmed ammonia and hydrogen desorption methods. High initial activity and selectivity of Ni 10 HAlBEA to hydrogen and carbon dioxide with unmodified BEA zeolite support in the steam reforming of ethanol reaction performed at 500°C was observed. However, fast deactivation of Ni 10 HAlBEA catalyst, manifested in the decrease of water conversion, drop of selectivity to H 2 and CO 2 , and increase in the selectivity to ethylene with the time-on-stream, was observed. In contrast, Ni 10 SiBEA zeolite catalyst showed lower initial activity but higher durability and resistance for carbon deposition. It was stated that dealumination of BEA zeolite led to the slight structural changes and simultaneously pronounced decrease of acidity. Formation of the large nickel crystallites was hindered on Ni 10 SiBEA zeolite catalyst. TEM and Raman spectroscopy studies indicated that deactivation of Ni 10 HAlBEA was related to formation of nickel mediated filamentous, graphitic and amorphous carbon deposits. Much smaller amounts of filamentous carbons were observed on the Ni 10 SiBEA zeolite catalyst prepared by the use of dealuminated zeolite support.

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Durability improvements of H-ZSM-5 zeolite for ethanol conversion after treatment with chelating agents

Cited by 12 publications

References 38 publications

Ethanol to Aromatics on Modified H‐ZSM‐5 Part I: Interdependent Dealumination Actions

Ethanol to Aromatics on Modified H‐ZSM‐5 Part I: Interdependent Dealumination Actions

Ethanol to Aromatics on Modified H‐ZSM‐5 Part II: An Unexpected Low Coking

Effects of dealumination on the performance of Ni-containing BEA catalysts in bioethanol steam reforming

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