An efficient microcapsule catalyst for one-step ethanol synthesis from dimethyl ether and syngas

Du, Ce; Hondo, Emmerson; Chizema, Linet Gapu; Ali, Riswan Hassan; Chang, Xiaoning; Dai, Lin; Ma, Qingxiang; Lu, Peng; Tsubaki, Noritatsu

doi:10.1016/j.fuel.2020.118971

Cited by 16 publications

(8 citation statements)

References 35 publications

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“…Furthermore, coaxial 3D printing technology can also integrate zeolites with different topologies and diverse metal oxides, which has been proven to be a versatile technique for compositing and constructing zeolite‐based core–shell structures. As illustration for the preparation, 3D‐FeMnO x @ZSM‐5 and 3D‐CuZnO x @MOR monoliths with tailorable geometries were 3D printed, which could be used for Fischer–Tropsch synthesis [ 44 ] and ethanol synthesis from dimethyl ether and syngas, [ 45 ] respectively (Figure S22, Supporting Information). The obtained 3D‐FeMnO x @ZSM‐5 and 3D‐CuZnO x @MOR monoliths with honeycomb shape (Figure 5e,g) exhibit complete core–shell structure from the cross‐section view of SEM images (Figure 5f,h and Figures S23 and S24, Supporting Information).…”

Section: Resultsmentioning

confidence: 99%

“…Preparation of 3D-CuZnO x @MOR: The conventional co-precipitation approach was used to prepare CuZnO x powder (Figure S26a, Supporting Information). [45] To obtain CuZnO x ink, CuZnO x (1.7 g), HNTs (0.3 g), and appropriate amount of 2% HPMC aqueous were mixed and stirred for 30 min. Commercial MOR zeolite (1.7 g, Figure S26b, Supporting Information, Nankai Catalyst Corporation, China), HNTs (0.3 g), and 2% HPMC aqueous (2 g) were stirred for 30 min to get MOR zeolite ink.…”

Section: Methodsmentioning

confidence: 99%

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Coaxial 3D Printing of Zeolite‐Based Core–Shell Monolithic Cu‐SSZ‐13@SiO₂ Catalysts for Diesel Exhaust Treatment

et al. 2023

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Core–shell catalysts with functional shells can increase the activity and stability of the catalysts in selective catalytic reduction of NOx with ammoniax. However, the conventional approaches based on multistep fabrication for core–shell structures encounter persistent restrictions regarding strict synthesis conditions and limited design flexibility. Herein, a facile coaxial 3D printing strategy is for the first time developed to construct zeolite‐based core–shell monolithic catalysts with interconnected honeycomb structures, in which the hydrophilic noncompact silica serves as shell and Cu‐SSZ‐13 zeolite acts as core. Compared to a Cu‐SSZ‐13 monolith which suffers from the interfacial diffusion, the SiO2 shell layer can increase the accessibility of active sites over Cu‐SSZ‐13@SiO2, resulting in a 10–20% higher NO conversion at200−550 °C under 300 000 cm3 g−1 h−1. Meanwhile, a thicker SiO2 shell enhances the hydrothermal stability of the aged catalyst by inhibiting the dealumination and the formation of CuOx. Other representative monolithic catalysts with different topological zeolites as shell and diverse metal oxides as the core can be also realized by this coaxial 3D printing. This strategy allows multiple porous materials to be directly integrated, which allows for flexible design and fabrication of various core–shell monolithic catalysts with customized functionalities.

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Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Coaxial 3D Printing of Zeolite‐Based Core–Shell Monolithic Cu‐SSZ‐13@SiO₂ Catalysts for Diesel Exhaust Treatment

et al. 2023

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“…The results indicated that core− shell catalyst prepared with Cu/ZnO as core and Cu-MOR as shell demonstrated outstanding selectivity of 45.9% for ethanol. 118 Their increased proximity between the acid sites and the metal further reduced coking resulting in remarkable stability for the catalyst. Similar work was investigated for direct syngas conversion to ethanol over RhMn and S-1 catalysts.…”

Section: Effects Ofmentioning

confidence: 99%

“…Du et al investigated a series of Cu, -MOR composite catalysts prepared as impregnated catalysts and core–shell catalysts to synthesize ethanol for syngas and DME. The results indicated that core–shell catalyst prepared with Cu/ZnO as core and Cu-MOR as shell demonstrated outstanding selectivity of 45.9% for ethanol . Their increased proximity between the acid sites and the metal further reduced coking resulting in remarkable stability for the catalyst.…”

Section: Syngas To Oxygenatesmentioning

confidence: 99%

Tandem Reactions over Zeolite-Based Catalysts in Syngas Conversion

et al. 2022

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Syngas conversion can play a vital role in providing energy and chemical supplies while meeting environmental requirements as the world gradually shifts toward a net-zero. While prospects of this process cannot be doubted, there is a lingering challenge in distinct product selectivity over the bulk transitional metal catalysts. To advance research in this respect, composite catalysts comprising traditional metal catalysts and zeolites have been deployed to distinct product selectivity while suppressing side reactions. Zeolites are common but highly efficient materials used in the chemical industry for hydroprocessing. Combining the advantages of zeolites and some transition metal catalysts has promoted the catalytic production of various hydrocarbons (e.g., light olefins, aromatics, and liquid fuels) and oxygenates (e.g., methanol, dimethyl ether, formic acid, and higher alcohols) from syngas. In this outlook, a thorough revelation on recent progress in syngas conversion to various products over metal-zeolite composite catalysts is validated. The strategies adopted to couple the metal species and zeolite material into a composite as well as the consequential morphologies for specific product selectivity are highlighted. The key zeolite descriptors that influence catalytic performance, such as framework topologies, proximity and confinement effects, acidities and cations, pore systems, and particle sizes are discussed to provide a deep understanding of the significance of zeolites in syngas conversion. Finally, an outlook regarding challenges and opportunities for syngas conversion using zeolite-based catalysts to meet emerging energy and environmental demands is also presented.

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“…However, this indirect route suffers from multiple processes and high energy consumptionin particular, the product separation for each process. In recent years, the direct synthesis of ethanol from DME and syngas over catalyst combinations of layer-by-layer and physical mixture or capsule catalysts has been proposed (Figure , Route D). − H–MOR was used for DME carbonylation, and Cu-based catalysts worked for MA hydrogenation during the reaction. However, the ethanol selectivity was typically limited at 40–49%, since ethanol and methanol were simultaneously produced in a molar ratio of 1:1 by MA hydrogenation.…”

Section: Introductionmentioning

confidence: 99%

Selective Transformation of Methanol to Ethanol in the Presence of Syngas over Composite Catalysts

et al. 2022

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The direct synthesis of ethanol from methanol via precise C–C coupling is a highly attractive but challenging target. Herein, we report the selective production of ethanol from methanol in the presence of syngas (CO/H2) by tandem catalysis over composite catalysts composed of mordenite (H–MOR) zeolite coated by carbon layer (H–MOR–DA@C) and Pt–Sn/CNT. This tandem route starts from methanol carbonylation with CO to acetic acid over H–MOR–DA@C, followed by acetic acid hydrogenation to ethanol over Pt–Sn/CNT. The selectivity of ethanol reached up to 60% with a CH3OH conversion of 98%. As compared to the H–MOR–DA matrix, the side reaction of ethanol dehydration to ethylene is effectively hindered over composite catalysts with H–MOR–DA coated by carbon layer. The special “carbon nest” with oxygenated functional groups such as ester or carboxylic acid, existing on the surface of H–MOR–DA@C, is crucial to preventing ethanol from dehydration, and thus improves the ethanol selectivity and catalytic stability. This work offers an effective strategy for direct synthesis of ethanol from methanol and design of efficient composite catalysts for tandem catalysis by controlling the reaction pathway.

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An efficient microcapsule catalyst for one-step ethanol synthesis from dimethyl ether and syngas

Cited by 16 publications

References 35 publications

Coaxial 3D Printing of Zeolite‐Based Core–Shell Monolithic Cu‐SSZ‐13@SiO₂ Catalysts for Diesel Exhaust Treatment

Coaxial 3D Printing of Zeolite‐Based Core–Shell Monolithic Cu‐SSZ‐13@SiO₂ Catalysts for Diesel Exhaust Treatment

Tandem Reactions over Zeolite-Based Catalysts in Syngas Conversion

Selective Transformation of Methanol to Ethanol in the Presence of Syngas over Composite Catalysts

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An efficient microcapsule catalyst for one-step ethanol synthesis from dimethyl ether and syngas

Cited by 16 publications

References 35 publications

Coaxial 3D Printing of Zeolite‐Based Core–Shell Monolithic Cu‐SSZ‐13@SiO2 Catalysts for Diesel Exhaust Treatment

Coaxial 3D Printing of Zeolite‐Based Core–Shell Monolithic Cu‐SSZ‐13@SiO2 Catalysts for Diesel Exhaust Treatment

Tandem Reactions over Zeolite-Based Catalysts in Syngas Conversion

Selective Transformation of Methanol to Ethanol in the Presence of Syngas over Composite Catalysts

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Product

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Coaxial 3D Printing of Zeolite‐Based Core–Shell Monolithic Cu‐SSZ‐13@SiO₂ Catalysts for Diesel Exhaust Treatment

Coaxial 3D Printing of Zeolite‐Based Core–Shell Monolithic Cu‐SSZ‐13@SiO₂ Catalysts for Diesel Exhaust Treatment