Syngas production via steam reforming of bioethanol over Ni–BEA catalysts: A BTL strategy

Rossetti, Ilenia; Compagnoni, Matteo; Finocchio, Elisabetta; Ramis, Gianguido; Michele, Alessandro Di; Zucchini, Azzurra; Dźwigaj, Stanisław

doi:10.1016/j.ijhydene.2016.07.149

Cited by 28 publications

(35 citation statements)

References 50 publications

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“…The Si/Al ratio of the samples increased as expected due to dealumination ( The A-phase was always the most abundant (46-56 wt%), followed by the B and C polymorphs (25-30% and 20-25%, respectively) [30]. No correlation between phase composition and sample treatment, dealumination and Ni loading was evidenced.…”

Section: -Textural Structural and Morphological Properties Of The Frmentioning

confidence: 68%

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Ethylene production via catalytic dehydration of diluted bioethanol: A step towards an integrated biorefinery

Rossetti

Compagnoni

Finocchio

et al. 2017

Applied Catalysis B: Environmental

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After a preliminary thermodynamic investigation, proper operating conditions have been selected to maximise ethylene productivity by ethanol dehydration and limit side products such as coke and higher olefins or oxygenates. We focused on the possibility to operate with a diluted bioethanol solution (ca. 50 wt%), which represents a promising and convenient raw material, obtainable by simple flash concentration of the fermentation broth. Furthermore, water addition to the ethanol dehydration reactor may help preventing catalyst coking and diethyl ether formation, although affecting the thermodynamic products distribution. A proof of concept for an ethanol dehydration process using diluted ethanol is also provided through process simulation. Catalysts based on a BEA zeolite have been compared, characterised by different acidity imparted by dealumination treatments. Ni addition in variable loading helped suppressing undesired byproducts, difficult to separate from ethylene. For instance, no trace of diethyl ether nor acetaldehyde has been observed for the Ni-loaded samples under optimised working conditions. Catalyst characterisation by FT IR allowed correlating a high selectivity to ethylene with the acid sites nature of the catalyst, whereas the presence of extraframework Lewis acidic sites induced faster coke formation. Durability was finally checked on the most active and selective catalyst evidencing stable operation for 80 h-on-stream and without evidence of coke deposition, as determined after characterisation of the spent samples. A γ-Al2O3 catalyst has been tested as benchmark under the same conditions

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Section: -Textural Structural and Morphological Properties Of The Frmentioning

confidence: 68%

“…Ni species more dispersed and strongly interacting with the support, as better detailed elsewhere [30]. This would limit the sintering expected after high temperature treatment.…”

Section: -Textural Structural and Morphological Properties Of The Frmentioning

confidence: 92%

Ethylene production via catalytic dehydration of diluted bioethanol: A step towards an integrated biorefinery

Rossetti

Compagnoni

Finocchio

et al. 2017

Applied Catalysis B: Environmental

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“…As the complexity of the reactions carried out in the process increases, this becomes one of the key issues to be settled prior to process design. In the following, we will consider the emblematic case of ethanol valorization into hydrogen or ethylene, as a pathway to the biorefinery exploitation [18][19][20][21]. In this view, a biomass-derived raw material is used to provide important chemicals/fuels in a more sustainable way.…”

Section: Processes Following Complex Kinetic Schemesmentioning

confidence: 99%

Process Simulation for the Design and Scale Up of Heterogeneous Catalytic Process: Kinetic Modelling Issues

et al. 2017

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Abstract:Process simulation represents an important tool for plant design and optimization, either applied to well established or to newly developed processes. Suitable thermodynamic packages should be selected in order to properly describe the behavior of reactors and unit operations and to precisely define phase equilibria. Moreover, a detailed and representative kinetic scheme should be available to predict correctly the dependence of the process on its main variables. This review points out some models and methods for kinetic analysis specifically applied to the simulation of catalytic processes, as a basis for process design and optimization. Attention is paid also to microkinetic modelling and to the methods based on first principles, to elucidate mechanisms and independently calculate thermodynamic and kinetic parameters. Different case studies support the discussion. At first, we have selected two basic examples from the industrial chemistry practice, e.g., ammonia and methanol synthesis, which may be described through a relatively simple reaction pathway and the relative available kinetic scheme. Then, a more complex reaction network is deeply discussed to define the conversion of bioethanol into syngas/hydrogen or into building blocks, such as ethylene. In this case, lumped kinetic schemes completely fail the description of process behavior. Thus, in this case, more detailed-e.g., microkinetic-schemes should be available to implement into the simulator. However, the correct definition of all the kinetic data when complex microkinetic mechanisms are used, often leads to unreliable, highly correlated parameters. In such cases, greater effort to independently estimate some relevant kinetic/thermodynamic data through Density Functional Theory (DFT)/ab initio methods may be helpful to improve process description.

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“…Besides, Pires et al 15 studied the reaction time of dealumination in solid state for Y zeolite and observed that after 2 h of reaction, parallel reactions with complex mechanisms could be responsible for the increase in Si/Al ratio, porosity and hydrophobicity. Nash et al 16 suggested that Brønsted acidic sites are more active than Lewis acidic sites for ethylene with an alcohol feed mixture for dehydration reaction in the following order: HZSM-5 > SAPO-34 > Al-MCM-41 > Zr- BEA zeolite presents high adsorptive capacity, which makes it much studied in several applications in catalysis [17][18][19] and selective adsorption/desorption of molecules, [20][21][22] but the dealumination process is less explored. Thus, in the current work, we disclose the beneficial effect of post-synthetic solid-state dealumination of BEA zeolite to generate hierarchical zeolitic structures within the crystallites for the dehydration of ethanol.…”

Section: Introductionmentioning

confidence: 99%

Catalytic Transformation Conditions of Ethanol on Dealuminated BEA Zeolites

Clemente¹,

Valadares²,

Lacava³

et al. 2019

J. Braz. Chem. Soc.

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Catalysis is an important tool in obtaining a range of derivative products from renewable sources, such as ethanol. Solid-state dealumination using ammonium hexafluorosilicate on the BEA zeolite under the treatment at temperature of 190 °C, 70 mol% dealumination in the presence of humidity and washing with buffer solution at 25 °C generated larger pores. The absence of washing procedure for the same sample resulted in pore blockage. Ethanol dehydration reactions showed conversion of 72% (64% ethylene and 8% diethyl ether) for this sample at 300 °C and high weight hourly space velocity (WHSV, 3247 h-1), whereas, at the same temperature but at a low WHSV (57 h-1), the conversion was 88% (49% ethylene and 39% diethyl ether). Dealuminated BEA zeolite presented better diffusion conditions, higher hydrophobicity and generated larger pores. Impregnation with H 3 PW 12 O 40 , H 4 SiW 12 O 40 and Nb 2 O 5 explained the selectivity, showing that Lewis acid sites from Nb 2 O 5 favored the diethyl ether production.

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Syngas production via steam reforming of bioethanol over Ni–BEA catalysts: A BTL strategy

Cited by 28 publications

References 50 publications

Ethylene production via catalytic dehydration of diluted bioethanol: A step towards an integrated biorefinery

Ethylene production via catalytic dehydration of diluted bioethanol: A step towards an integrated biorefinery

Process Simulation for the Design and Scale Up of Heterogeneous Catalytic Process: Kinetic Modelling Issues

Catalytic Transformation Conditions of Ethanol on Dealuminated BEA Zeolites

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