Influence of Tandem Catalysis and Optimised Parameters on Syngas-Dimethyl Ether Co-fed Process for Ethanol Direct Synthesis in a Dual Bed Reactor

Lu, Peng; Hondo, Emmerson; Chizema, Linet Gapu; Lu, Chao; Mei, Yongfei; Tong, Ming‐Liang; Xing, Chuang; Yang, Renqiang

doi:10.1007/s10562-019-02890-9

Cited by 14 publications

(13 citation statements)

References 41 publications

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“…XRD analysis was conducted to identify the crystallinity of all catalysts samples, which included metal CZZA, Mix‐CZZA−H‐β, pure H‐β zeolite and CZZA@H‐β‐P‐3 as shown in Fig 1. As can be visibly noticed, the pattern of CZZA catalyst exhibited characteristic peaks of both CuO mainly as tenorite (JCPDS 48‐1548) and ZnO as zincite (JCPDS 36‐1451) . It was reported that an intrinsic association between CuO and ZnO species enhances particle dispersion, where ZnO species functions as spacers between metallic Cu particles inhibiting them from aggregation and sintering …”

Section: Resultsmentioning

confidence: 99%

LPG Direct Synthesis from Syngas over a Cu/ZnO/ZrO₂/Al₂O₃@H‐β Zeolite Capsule Catalyst Prepared by a Facile Physical Method

Hondo

Chizema

et al. 2020

ChemistrySelect

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Liquid Petroleum Gas has recently captured great attention worldwide due to the escalating demand for non‐oil eco‐friendly fuel resources. However, the catalytic synthesis process still possesses some thermodynamic and raw material conversion flaws, in addition to unfavorable occurrence of side reactions. Herein, we present an advanced core‐shell hybrid catalyst, facilely prepared by the physical coating method, promoting not only high product yield, but also effectively eliminating design limitations accrued on employing the hydrothermal synthesis technique. The designed capsule catalyst, named CZZA@H‐β‐P‐3, has Cu/ZnO/ZrO2/Al2O3 (CZZA) catalyst as core and H‐β zeolite as shell. CZZA@H‐β‐P‐3 capsule catalyst was then used for direct synthesis of liquefied petroleum gas from syngas. A general mixture catalyst, Mix‐CZZA−H‐β, was used for comparison under same conditions. XRD, SEM‐EDS and NH3‐TPD characterization techniques were utilized to probe the extrinsic/intrinsic properties of the as‐prepared catalysts. CZZA@H‐β‐P‐3 exhibited excellent activity, in comparison. At optimal conditions, CZZA@H‐β‐P‐3 increased CO conversion from 40.94 % to 54.8 %, and LPG selectivity from 17.01 % to 26.04 %. Dimethyl ether (DME) selectivity decreased to zero. The excellent catalytic activity displayed on CZZA@H‐β‐P‐3 capsule catalyst was credited to the special core‐shell structure constructed from highly synergetic materials with a confined reaction affection, which uniquely accelerated syngas conversion to LPG.

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Section: Resultsmentioning

confidence: 99%

LPG Direct Synthesis from Syngas over a Cu/ZnO/ZrO₂/Al₂O₃@H‐β Zeolite Capsule Catalyst Prepared by a Facile Physical Method

Hondo

Chizema

et al. 2020

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“…H-type mordenite was synthesized using the hydrothermal synthesis procedure, then carefully modified with an appropriate amount of copper using the incipient wetness impregnation method, as reported in our recent work …”

Section: Experimental Sectionmentioning

confidence: 99%

“…All fresh catalysts were mixed with a small amount (up to 0.1 g) of inert carborundum (SiC) as diluent and for ascertaining isothermal conditions on catalyst beds. Catalyst arrangement and pretreatment in the dual bed reactor, product discharge, detection, and computational evaluation were conducted as have been reported in our previous work . For substantiation purposes, experiments for the as-prepared catalysts were conducted three times, and the results were averaged.…”

Section: Experimental Sectionmentioning

confidence: 99%

“…In the same line, use of pressurized materials with high volatility such as syngas and other high energy compounds like dimethyl ether (DME) still pose transportation and storage complexities, despite being green; hence, generating stable liquid fuels with high energy turnover would be more ideal. EtOH is a liquid fuel with high sustainability and less toxicity hence comparably easier in handling, transportation, and storage, in addition to constituting a remarkable energy density of about 25 MJ·Kg –1 . , An ethanol (EtOH) direct synthesis route from synthetic gas through DME carbonylation, over zeolite catalysts, ensued by methyl acetate (MA) hydrogenation, over some ternary metal oxide catalyst (CuO/ZnO/Al 3 O 2 ), in a single catalytic dual bed reactor, is a promising high carbon efficiency technology as recently reported. − …”

Section: Introductionmentioning

confidence: 99%

“…Zeolite catalysts have been successfully modified with nonhalide metals such as Fe, Pt, Co, Cu, and so forth. − Despite excellent catalytic performance displayed by copper on HMOR (as in Cu-MOR) in recent reports during DME carbonylation, , catalyst deactivation due to Cu particle sintering during preparation and reaction processes has been a serious drawback, which equally limited recyclability of the catalyst due to high thermal treatment associated with the regeneration process. , Another unfortunate setback emanating from the aforementioned catalyst deactivation cult is the limited DME conversion which results in the overall dual bed reaction process favoring higher selectivity for the byproduct (methanol). DME carbonylation, which is the rate-determining step of the series reaction, is more difficult compared to MA hydrogenation.…”

Section: Introductionmentioning

confidence: 99%

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Developing Cu-MOR@SiO₂ Core–Shell Catalyst Microcapsules for Two-Stage Ethanol Direct Synthesis from DME and Syngas

Hondo

Chizema

et al. 2020

Ind. Eng. Chem. Res.

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Catalytic conversion of Syngas and dimethyl ether to ethanol is a green strategy of harnessing fine chemicals from nonpetroleum origins. In the process, catalyst deactivation coupled with higher byproduct selectivities is still a serious cause of concern due to inevitable yield losses. Herein, we synthesized highly ordered Cu-MOR@SiO2 core–shell microcapsules, employing a facile scalable surfactant-directed sol–gel technique. Comparably, the microcapsules displayed higher DME carbonylation (83.8%) activity and a remarkable product yield (48.7%). Furthermore, confinement of Cu-MOR particles surrounded by SiO2 crystals cushions dispersed Cu components from inevitable sintering during exposure to higher temperatures, paving way for an effective regeneration treatment. However, this catalyst will function in tandem with commercialized CZA catalyst in a dual bed reactor. The novel Cu-MOR@SiO2 encapsulated catalyst displayed a stable longer service life and higher product yield, thus providing the dual bed ethanol synthesis pathway from cofeeding dimethyl ether and syngas, an opportunity toward commercial production.

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Insights Into the one‐Step Dimethyl Ether Carbonylation to Ethanol Over Cu/ZnO@Cu‐MOR Core‐Shell Catalysts with Porogen Engagement

Lu,

Nyako,

Lin

et al. 2024

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This study investigates the one‐step ethanol synthesis from dimethyl ether and syngas using the catalysts combining Cu/ZnO oxides and modified Cu‐MOR zeolite. In addition to physically mixed two‐component catalysts, multifunctional catalysts featuring a Cu/ZnO core and modified zeolite (Cu‐MOR and HMOR) shell are also presented. Further, the porogenic agent of dihexadecyldimethylammonium bromide (DHAB) was involved in the synthesis process of the MOR zeolite components of Cu/ZnO@Cu‐MOR and Cu/ZnO/Cu‐MOR catalysts, but not in that of Cu/ZnO@Cu‐MOR° catalyst. A series of characterization measures including XRD, TGA, BET, SEM, TEM and EDS have been systematically studied on the prepared catalysts. Characterizations of the catalyst surface structure and texturing parameters revealed a disturbance in crystallinity upon Cu insertion, facilitating syngas separation and promoting DME carbonylation while preventing undesired CO hydrogenation. The addition of DHAB as a porogen in the synthesis of zeolite shell improved specific surface area and porosity of zeolite shell, and reduced coke deposition, without leaching active metal components, resulting in enhanced reaction properties. Cu/ZnO@Cu‐MOR core‐shell catalyst showed good performance with 28.9 % DME conversion and 43.8 % selectivity for ethanol. The optimized pore structure and enhanced catalytic performance of the modification process validate the effectiveness and efficiency of this strategy.

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Influence of Tandem Catalysis and Optimised Parameters on Syngas-Dimethyl Ether Co-fed Process for Ethanol Direct Synthesis in a Dual Bed Reactor

Cited by 14 publications

References 41 publications

LPG Direct Synthesis from Syngas over a Cu/ZnO/ZrO₂/Al₂O₃@H‐β Zeolite Capsule Catalyst Prepared by a Facile Physical Method

LPG Direct Synthesis from Syngas over a Cu/ZnO/ZrO₂/Al₂O₃@H‐β Zeolite Capsule Catalyst Prepared by a Facile Physical Method

Developing Cu-MOR@SiO₂ Core–Shell Catalyst Microcapsules for Two-Stage Ethanol Direct Synthesis from DME and Syngas

Insights Into the one‐Step Dimethyl Ether Carbonylation to Ethanol Over Cu/ZnO@Cu‐MOR Core‐Shell Catalysts with Porogen Engagement

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Influence of Tandem Catalysis and Optimised Parameters on Syngas-Dimethyl Ether Co-fed Process for Ethanol Direct Synthesis in a Dual Bed Reactor

Cited by 14 publications

References 41 publications

LPG Direct Synthesis from Syngas over a Cu/ZnO/ZrO2/Al2O3@H‐β Zeolite Capsule Catalyst Prepared by a Facile Physical Method

LPG Direct Synthesis from Syngas over a Cu/ZnO/ZrO2/Al2O3@H‐β Zeolite Capsule Catalyst Prepared by a Facile Physical Method

Developing Cu-MOR@SiO2 Core–Shell Catalyst Microcapsules for Two-Stage Ethanol Direct Synthesis from DME and Syngas

Insights Into the one‐Step Dimethyl Ether Carbonylation to Ethanol Over Cu/ZnO@Cu‐MOR Core‐Shell Catalysts with Porogen Engagement

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Product

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About

LPG Direct Synthesis from Syngas over a Cu/ZnO/ZrO₂/Al₂O₃@H‐β Zeolite Capsule Catalyst Prepared by a Facile Physical Method

LPG Direct Synthesis from Syngas over a Cu/ZnO/ZrO₂/Al₂O₃@H‐β Zeolite Capsule Catalyst Prepared by a Facile Physical Method

Developing Cu-MOR@SiO₂ Core–Shell Catalyst Microcapsules for Two-Stage Ethanol Direct Synthesis from DME and Syngas