Effects of the support on bifunctional one-step synthesis of methylal <i>via</i> methanol oxidation catalysed by Fe–Mo-based bifunctional catalysts

Yuan, Meng; Tang, Rongjun; Sun, Xiangyu; Zhang, Zhimei; Tian, Yuanyu; Qiao, Yingyun

doi:10.1039/d0se01194k

Cited by 9 publications

(6 citation statements)

References 52 publications

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“…The discussion of thermodynamics, kinetics, and reaction mechanism is carried out on the basis of previous research, so the preparation method of the catalyst is consistent with the previous preparation method. Mo‐Fe/CAR catalysts with different carriers and optimized Mo‐Fe‐based bifunctional catalysts were selected for experimental validation (see the Supplementary Material for details of the specific preparation method) 34 …”

Section: Methodsmentioning

confidence: 99%

“…Mo-Fe/ CAR catalysts with different carriers and optimized Mo-Fe-based bifunctional catalysts were selected for experimental validation (see the Supplementary Material for details of the specific preparation method). 34…”

Section: Catalyst Preparationmentioning

confidence: 99%

“…36 Investigate the relationship between thermodynamic kinetics and product distribution in the laboratory mini-fluidized bed reactor (The eaction device and experimental methods are described in detail in Supplementary Material). 34 Methanol, DMM, FA, methyl formate(MF), and dimethyl ether(DME) are detected in the FID detector with SE-56 capillary column chromatograph (40 m Â 0.25 mm Â 0.25 μm). CO x and O 2 are analysed using packed columns with TCD detectors.…”

Section: Thermodynamics Kinetics and Reaction Mechanism Evaluationmentioning

confidence: 99%

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One‐step synthesis of methylal via methanol oxidation: Reaction kinetics, mechanism, thermodynamics, and product analysis

Yuan

Sun

Tian

et al. 2022

Intl J of Energy Research

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Summary The recent abundance of methanol has made it an attractive raw material for chemical synthesis. This study conducts a thermodynamic analysis of the main and side reactions in a system where methanol is oxidized to methylal. A relationship between the thermodynamics and product distribution of this system is proposed. By studying the effect of reaction temperature on the catalytic activity of a Mo‐Fe/HZSM‐5 (80‐80) catalyst, the relationship between thermodynamic parameters and product distribution was further verified. Kinetic analysis of the one‐step process shows that a lower activation energy is one of the reasons for the higher catalytic activity of the iron‐molybdenum‐based bifunctional catalyst. Accordingly, it is proposed that all main and side reactions in this process are driven by two chemical adsorption reactions. The first occurs at active sites of iron and molybdenum oxidation on the catalyst surface. The adsorbed methanol and O2 obtain hydroxyl and methoxy groups linked to the iron molybdate. Subsequently, desorbed formaldehyde and methanol undergo a second chemical adsorption on the acidic active centres of the catalyst with surface carbonyl and hydroxyl groups, respectively. Formaldehyde and the adsorbed methoxy group are catalysed by the acidic sites to generate intermediates similar to the methoxy and methylene group structures. This study provides complete information on the thermodynamics, kinetics, and reaction mechanism of a one‐step process of producing methylal from methanol, thereby allowing optimization of this process.

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Section: Methodsmentioning

confidence: 99%

Section: Catalyst Preparationmentioning

confidence: 99%

Section: Thermodynamics Kinetics and Reaction Mechanism Evaluationmentioning

confidence: 99%

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One‐step synthesis of methylal via methanol oxidation: Reaction kinetics, mechanism, thermodynamics, and product analysis

Yuan

Sun

Tian

et al. 2022

Intl J of Energy Research

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“…En general, este tipo de catalizadores presentan un buen desempeño en términos de selectividad hacia formaldehido (alrededor del 94%) y conversión de metanol (alrededor del 99%). Adicionalmente, se ha observado a nivel industrial la generación de pequeñas cantidades de OME 1 como subproducto, lo que evidencia la presencia de una funcionalidad acida, la cual es susceptible de ser mejorada para incrementar la productividad de 1,1-dimetoximetano 13,26 .…”

Section: Referenciasunclassified

Hacia el desarrollo de alternativas sostenibles al combustible diésel: síntesis de 1,1-dimetoximetano (OME1) a través de catálisis bifuncional

Herrera,

Rodriguez

2023

Rev. Quim.

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Disminuir el impacto ambiental derivado del uso de combustibles fósiles necesita el desarrollo de fuentes de energía renovables, y la producción sostenible de combustibles líquidos. Los éteres de oximetileno (OMEs), son compuestos oxigenados que han surgido como una potencial alternativa para sustituir el combustible Diesel. El uso de estos éteres en los motores disminuye la formación de hollín y óxidos de nitrógeno (NOx) durante la combustión. Dentro de esta familia de compuestos, el 1,1-dimetoximetano (OME1) tiene especial interés, no solo por su uso como solvente industrial o como intermediario químico, sino, también porque puede ser usado como materia prima para la producción de OMEs de cadena larga. La síntesis directa de OME1 involucra la oxidación selectiva de metanol sobre catalizadores bifuncionales, los cuales han sido objeto de estudio durante las últimas décadas. Este trabajo resume las principales características de los distintos sistemas catalíticos desarrollados, los cuales juegan un papel fundamental para la producción comercial del 1,1-dimetoximetano.

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“…Additionally, the methyl ether peak intensity of the Fe-Mo/ZSM-5 catalyst with Si:Al = 40 was greater than that of the Fe-Mo/ZSM-5 catalyst with Si:Al = 60. In previous studies 37 (adapted from ref. 9), our team revealed that the tetrahedral coordination of Al provided Bronsted acid (B acid) sites and Lewis acid (L acid) sites on the Si-Al framework.…”

Section: In-situ Infrared Exploration Of Reaction Mechanismmentioning

confidence: 99%

Reaction mechanisms and catalysis in the one-step synthesis of methylal via methanol oxidation

Yuan¹,

Dong²,

Tian³

et al. 2021

Preprint

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This paper reports on the scaling-up of a one-step methanol production process from the laboratory scale to the pilot scale. This lays the foundation for the industrialization of a one-step process for preparing DMM from methanol. After a long period of operation in the circulating fluidized bed, the Fe-Mo/HZSM-5 catalyst was shown to have high stability and carbon deposition resistance, and the regeneration effect of the circulating regeneration fluidized bed was better. In addition, in-situ DRIFTS was used to explore the effects of reaction time, the Mo-Fe ratio and carrier Si-Al ratio on the reaction and product distribution. It was found that the synergistic effect of oxidation centers and acid centers was the fundamental reason for the excellent catalytic performance of the Fe-Mo/HZSM-5 catalyst. And proposed the reaction mechanisms in the one-step synthesis of methylal via methanol oxidation.

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Effects of the support on bifunctional one-step synthesis of methylal via methanol oxidation catalysed by Fe–Mo-based bifunctional catalysts

Abstract: In the one-step preparation of methylal from methanol, achieving high methanol conversion and high methylal yield is a huge challenge. To address this problem, in this study a new Mo:Fe(2)/CAR...

Cited by 9 publications

References 52 publications

One‐step synthesis of methylal via methanol oxidation: Reaction kinetics, mechanism, thermodynamics, and product analysis

One‐step synthesis of methylal via methanol oxidation: Reaction kinetics, mechanism, thermodynamics, and product analysis

Hacia el desarrollo de alternativas sostenibles al combustible diésel: síntesis de 1,1-dimetoximetano (OME1) a través de catálisis bifuncional

Reaction mechanisms and catalysis in the one-step synthesis of methylal via methanol oxidation

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