Direct dimethyl ether synthesis from syngas on copper–zeolite hybrid catalysts with a wide range of zeolite particle sizes

Herein, kinetic modelling and kinetic parameters were used to study methanol dehydration to dimethyl ether reaction and revealed that the best model to fit the experimental data was the Bercic model. The dehydration reaction undergoes dissociative adsorption Langmuir-Hinshelwood mechanism of methanol on the alumina catalyst surface, with the calculated value of the activation energy was 136.7 kJ mol −1 . Moreover, the effect of different kinetic parameters such as the catalyst weight and methanol concentration or water in the feed on the catalytic performance of η-Al 2 O 3 was examined in a fixed bed reactor under the reaction conditions where the temperature ranged from 180 to 350 °C with a WHSV = 12.1 h −1 . Graphical Abstract

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“…1) or via the dehydration of methanol over solid catalysts such as Al 2 O 3 (Eq. 2), according to the following reactions [1][2][3][4][5][6]:…”

Section: Introductionmentioning

confidence: 99%

Kinetic Investigation of η-Al2O3 Catalyst for Dimethyl Ether Production

Osman

Abu‐Dahrieh

2018

Catal Lett

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“…Nowadays, dimethyl ether (DME) has attracted more and more attention concerning its application acting as both an industrially important chemical materials and a clean alternative fuel. [1][2][3][4][5] DME was generally produced by two routes: one is methanol dehydration catalyzed by an acidic catalyst, in which methanol is previously synthesized by catalyzed hydrogenation of syngas; the other is a direct synthesis route from one-pot transformation of syngas over a bifunctional catalyst. [5][6][7][8][9][10][11] The latter is regarded as a promising pathway for DME production.…”

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confidence: 99%

Implanting Copper−Zinc Nanoparticles into the Matrix of Mesoporous Alumina as a Highly Selective Bifunctional Catalyst for Direct Synthesis of Dimethyl Ether from Syngas

Sun

Zhao

2020

ChemCatChem

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Dimethyl ether (DME) is an industrially important intermediate and clean alternative fuel. Thus, developing an efficient bifunctional catalyst for syngas‐to‐DME is practically important but remains a challenge. In this paper, a copper−zinc implanting into matrix of mesoporous alumina (CuZn@m−Al2O3) catalyst was prepared by introducing the as‐prepared Cu−Zn oxalate nanoparticles into the Al(i‐OPr)3‐containing precursor solution for preparing mesoporous Al2O3 (m‐Al2O3) through evaporation‐inducing assembly method. The preparation of Cu−Zn oxalate in advance for synthesizing CuZn@m−Al2O3 can intensify the Cu−ZnO interaction, confirmed by XRD and H2‐TPR. Thanks to the unique CuZn‐implanting closed structure, CuZn@m−Al2O3 shows 89.0 % of higher selectivity with comparable CO conversion (15.5 %) than the previously reported supported‐type CuZn catalyst on m‐Al2O3 (CuZn/m−Al2O3, 75.2 %) for hydrogenation of syngas to DME. Over the developed CuZn@m−Al2O3 catalyst, 0.16 mmol g−1 cat h−1 of high DME rate can be achieved. CuZn@m−Al2O3 also shows higher methanation resistance (2.7 % CH4) compared to CuZn/m−Al2O3 (6.3 %), ascribed to intensified Cu−Zn interaction owing to the as‐formation of Cu−Zn oxalate in advance. Moreover, Both CuZn@m−Al2O3 and CuZn/m−Al2O3 exhibit high stability. The outstanding catalytic performance of CuZn@m−Al2O3 allows it to be a promising catalyst for DME synthesis from syngas.

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“…[2][3][4][21][22][23][24][25][26][27][28][29][30] The hybrid catalysts prepared by physically mixing methanol synthesis catalyst (CuÀ ZnOÀ Al 2 O 3 ) and methanol dehydration catalyst (solid acid) were attempted to catalyze the STD process. [31][32][33][34][35][36][37][38][39][40] The methanol synthesis unit in the hybrid catalysts have been focused on tuning catalysts composition, [21][22][23][24][25] synthetic method, [26,27] preparation parameters of Cu-based catalysts [28,29] and alternatives to Cu-based. [30] The methanol dehydration unit in the hybrid catalysts has been focused on the modulation of particle size, [31] structure [32][33][34] and modification of acidic sites by metal [35][36][37][38] of zeolite and γ-Al 2 O 3 .…”

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confidence: 99%

“…[31][32][33][34][35][36][37][38][39][40] The methanol synthesis unit in the hybrid catalysts have been focused on tuning catalysts composition, [21][22][23][24][25] synthetic method, [26,27] preparation parameters of Cu-based catalysts [28,29] and alternatives to Cu-based. [30] The methanol dehydration unit in the hybrid catalysts has been focused on the modulation of particle size, [31] structure [32][33][34] and modification of acidic sites by metal [35][36][37][38] of zeolite and γ-Al 2 O 3 . [27][28][29]39,40] Especially, HZSM-5 has been considered as an excellent candidate for methanol dehydration.…”

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confidence: 99%

“…[27][28][29]39,40] Especially, HZSM-5 has been considered as an excellent candidate for methanol dehydration. [31][32][33][34][35][36][37][38] In addition, reaction conditions, [41][42][43][44][45][46][47][48] catalyst regeneration [49] and interaction between different functional components [50] have also been investigated. However, some deficiencies still exist in STD process over the hybrid catalyst.…”

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confidence: 99%

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Ethanol as a Binder to Fabricate a Highly‐Efficient Capsule‐Structured CuO−ZnO−Al₂O₃@HZSM‐5 Catalyst for Direct Production of Dimethyl Ether from Syngas

Guo

Zhao

2020

ChemCatChem

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This work reports a highly efficient capsule‐structured CuO−ZnO−Al2O3@HZSM‐5 (CZA@HZSM‐5‐EtOH) core‐shell catalyst for the direct conversion of syngas to dimethyl ether by a facile physical coating method with ethanol as a binder through coating micrometer‐sized HZSM‐5 shell on the prior‐shaped millimeter‐sized CZA core, it shows 2.9 times higher CO conversion with the 2.7 times higher turnover frequency and 9.2 times higher dimethyl ether space‐time yield of the CZA@HZSM‐5‐SS catalyst prepared by a similar process but with silica sol as a binder (315.5 vs 34.3 gDME kgcat−1 h−1). The relationship between the structure and performance was explored by a variety of characterization techniques including X‐ray diffraction (XRD), scanning electron microscope (SEM), energy dispersive spectrometer (EDS), X‐ray diffraction (XRD), ammonia temperature programmed desorption (NH3‐TPD), nitrogen adsorption‐desorption, H2‐temperature‐programmed reduction (H2‐TPR) and H2‐TPR after oxidation of the samples by N2O. CZA@HZSM‐5‐EtOH can be considered as a highly efficient and practical catalyst for dimethyl ether synthesis from syngas. This work presents a new avenue to design other bifunctional catalysts for the cascade reactions in which the raw materials can be converted into an intermediate over the core and then the as‐formed intermediate over the core can be subsequently converted into the final product.

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Direct dimethyl ether synthesis from syngas on copper–zeolite hybrid catalysts with a wide range of zeolite particle sizes

Cited by 78 publications

References 71 publications

Kinetic Investigation of η-Al2O3 Catalyst for Dimethyl Ether Production

Kinetic Investigation of η-Al2O3 Catalyst for Dimethyl Ether Production

Implanting Copper−Zinc Nanoparticles into the Matrix of Mesoporous Alumina as a Highly Selective Bifunctional Catalyst for Direct Synthesis of Dimethyl Ether from Syngas

Ethanol as a Binder to Fabricate a Highly‐Efficient Capsule‐Structured CuO−ZnO−Al₂O₃@HZSM‐5 Catalyst for Direct Production of Dimethyl Ether from Syngas

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Direct dimethyl ether synthesis from syngas on copper–zeolite hybrid catalysts with a wide range of zeolite particle sizes

Cited by 78 publications

References 71 publications

Kinetic Investigation of η-Al2O3 Catalyst for Dimethyl Ether Production

Kinetic Investigation of η-Al2O3 Catalyst for Dimethyl Ether Production

Implanting Copper−Zinc Nanoparticles into the Matrix of Mesoporous Alumina as a Highly Selective Bifunctional Catalyst for Direct Synthesis of Dimethyl Ether from Syngas

Ethanol as a Binder to Fabricate a Highly‐Efficient Capsule‐Structured CuO−ZnO−Al2O3@HZSM‐5 Catalyst for Direct Production of Dimethyl Ether from Syngas

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Ethanol as a Binder to Fabricate a Highly‐Efficient Capsule‐Structured CuO−ZnO−Al₂O₃@HZSM‐5 Catalyst for Direct Production of Dimethyl Ether from Syngas