Isothermal cyclic conversion of methane to methanol using copper-exchanged ZSM-5 zeolite materials under mild conditions

Burnett, Linda Andersson; Rysakova, M.; Wang, Ke; González-Carballo, Juan M.; Tooze, Robert P.; García-García, Francisco J.

doi:10.1016/j.apcata.2019.117272

Cited by 16 publications

(8 citation statements)

References 34 publications

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“…It should be noted that no other compounds besides MeOH were detected in the chromatographic analysis. The obtained amount of MeOH is in the same order of magnitude with those reported in the literature (Tomkins et al, 2016(Tomkins et al, , 2019Wulfers et al, 2015), but much less compared with cycling continuous flow processes (Álvarez et al, 2020;Burnett et al, 2019;Jovanovic et al, 2020;Ma et al, 2020). Likewise, a dependency on Cu wt % of catalyst was observed (Figure 1) with a similar tendency to the work reported by Le et al (2017) and Oord, Schmidt, and Weckhuysen (2018).…”

Section: Resultssupporting

confidence: 86%

“…MeOH is a very important raw material for the chemical industry, with an increasing demand for a wide variety of applications (Dalena et al, 2018;Hammond, Conrad, and Hermans, 2012). CH 4 is one of the most important fossil fuels in the planet, which is not fully exploited because of the economical unsuitability of the synthetic pathway from syngas to produce the required quantities of MeOH (Burnett et al, 2019;Jovanovic et al, 2020). Therefore, the direct conversion of CH 4 to MeOH has been a long-standing challenge in the field of catalysis (Tomkins, Ranocchiari, and van Bokhoven, 2017).…”

Section: Introductionmentioning

confidence: 99%

“…Thus, the search for catalysts and reaction conditions for this process is a topical issue. A wide variety of materials have been developed as catalysts for this reaction, including copper-exchanged zeolites and mordenite (Burnett et al, 2019;Lomachenko et al, 2019;Tomkins et al, 2016;Wulfers, Teketel, Ipek, and Lobo, 2015). These kinds of materials are synthesized from different copper precursors.…”

Section: Introductionmentioning

confidence: 99%

“…Copper mordenite has been reported as one of the most efficient inorganic materials, with applications in CH 4 to MeOH conversion under mild conditions (Álvarez, Marín, and Ordóñez, 2020;Burnett et al, 2019;Tomkins et al, 2016;Wulfers et al, 2015). Furthermore, it has been linked to the solid-state ion exchange synthesis method with a higher amount of MeOH production (Sainz-Vidal, Balmaseda, Lartundo-Rojas, and Reguera, 2014).…”

Section: Introductionmentioning

confidence: 99%

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Batch Conversion of Methane to Methanol Using Copper Loaded Mordenite: Influence of the Main Variables of the Process

Mojica¹,

González²,

Frómeta³

2021

Ing. Inv.

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Due to the demands of oxygenated derivatives of hydrocarbons for the industry, the methane (CH4) to methanol (MeOH) conversion through solid-state catalysis is a current topic, with definite questions and specific challenges. This work shows a statistical model that predicts the quantity of methanol produced through a batch conversion process employing copper-exchanged mordenite in accordance with a full factorial experimental design. Synthesis was performed through solid-state ion exchange from Cu(acac)2 and NH4-Mordenite, obtaining weight percentages (%Cu) of 1%, 3%, and 5%, which was followed by activation through calcination at a range of temperatures (Tcal) between 300-500 °C, as well as a reaction with methane under 2-10 bar pressure (P) in static conditions employing a batch reactor. The quantities of MeOH produced, and their yields were determined through a gas chromatography and mass spectrometry analysis of the reaction samples. Finally, the role and contribution of each of the variables considered in the conversion process were analyzed. By using a nonlinear model, a quadratic dependence with %Cu and P in the studied range of the variables was found, as well as a linear dependence with Tcal. Finally, for this experiment, the highest yields (µmol/g) were obtained with the following conditions: %Cu=3 %, P=6 bar, and Tcal=400 °C.

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Section: Resultssupporting

confidence: 86%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Batch Conversion of Methane to Methanol Using Copper Loaded Mordenite: Influence of the Main Variables of the Process

Mojica¹,

González²,

Frómeta³

2021

Ing. Inv.

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“…Naturally, binuclear copper- or iron-metal centers of methane monooxygenase (MMO) enzymes are able to oxidize the C–H bond of methane under ambient conditions. , Inspired by the MMO active sites, engineering of transition metal centers confined in zeolite (e.g., copper- and iron-exchanged ZSM-5) is of considerable interest in converting methane to methanol at moderate temperatures − because the binuclear metal centers can be stabilized by a zeolite framework. ,− Although there are the above-beneficial effects of zeolites for the conversion of methane to methanol, it is mandatory to combine with the further step of product extraction by using polar solvents such as water due to a strong interaction between the reaction intermediates and/or products and hydrophilic surfaces of zeolites. ,,− To circumvent this issue, the zeolite surface modification by hydrophobic moieties should be one of the most challenging aspects to increase the methanol yield.…”

Section: Introductionmentioning

confidence: 99%

Methane Utilization to Methanol by a Hybrid Zeolite@Metal–Organic Framework

Imyen

Znoutine

Suttipat

et al. 2020

ACS Appl. Mater. Interfaces

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The development of an effective approach for methane utilization, especially methane conversion to methanol, is a crucial challenge that has remained unsolved satisfactorily. Herein, we propose an alternative concept of methane utilization to methanol over Fe-ZSM-5@ZIF-8. The concept is to use the designed composite as a dual catalyst in which ZIF-8 and Fe-ZSM-5 act simultaneously as a gas adsorbent and catalyst, respectively. In this case, methane can be adsorbed on ZIF-8 at 50 °C and subsequently converted to methanol at a moderate temperature (150 °C) on Fe-ZSM-5. Interestingly, the promising catalytic performance is observed on Fe-ZSM-5@ZIF-8, whereas only trace amounts of produced methanol are detected on isolated Fe-ZSM-5 and ZIF-8. Moreover, the designed composite also facilitates a facile methanol desorption at the hydrophobic surface of the composite. This first example opens up new promising horizons in combined perspectives for gas storage and catalytic process applications.

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Applications of Zeolites to C1 Chemistry: Recent Advances, Challenges, and Opportunities

2020

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However, due to growing concerns regarding crude oil depletion and increasing environmental requirements, finding abundant fossil hydrocarbons with high H 2 /C ratios as well as alternative carbon resources has become crucial to maintaining sustainable, environmentally benign systems that can aid human development. [2] Thus, one-carbon (C1) chemistry, which is the chemistry of C1 molecules that can be derived from sources other than fossil hydrocarbons, including carbon monoxide (CO), carbon dioxide (CO 2), methane (CH 4), methanol (CH 3 OH), and formic acid (HCOOH), has emerged and plays important roles in the energy supply and high-value chemical preparation. [1,3] These C1 resources can be obtained from natural gas, shale gas, coal, biomass, solid wastes, and CO 2 emissions. [3a,4] Extensive studies have been dedicated to the catalytic conversion of C1 molecules, including production of dimethyl ether (DME) and liquid fuels from syngas (a mixture of CO and H 2); production of methanol, light olefins, and even aromatics from CH 4 ; and production of hydrogen from HCOOH. [5] All of these transformations require metallic catalytic species such as single atoms; clusters; or oxides, carbides, or alloy particles (e.g., Rh-, AuPd-, Fe 3 O 4-, and Fe 5 C 2-based catalysts). However, these isolated metallic species suffer from severe sintering due to a lack of confinement effects from supports, which leads to poor catalytic stability and decreased selectivities toward their target products. The efficient production of a specific range of hydrocarbons or oxygenates remains a difficult scientific and technical challenge. Overcoming product selectivity limitations and improving catalyst stabilities via catalyst designs are important areas of research. Zeolites are an important class of shape-selective catalysts with uniform micropores, tunable acidities, and high thermal and hydrothermal stabilities. Over the past decade, they have gained broad popularity and been applied to various industrially important catalytic processes. [6] In particular, the design and development of zeolite-based mono-, bi-, and multifunctional catalysts that combine the advantages of zeolites with those of metallic catalytic species have boosted the application of zeolites to C1 chemistry. As shown in Figure 1, value-added hydrocarbons and oxygenates can be produced from C1 molecules via various catalytic routes over zeolite-based catalysts. By May of 2020, the Structure Commission of the International C1 chemistry, which is the catalytic transformation of C1 molecules including CO, CO 2 , CH 4 , CH 3 OH, and HCOOH, plays an important role in providing energy and chemical supplies while meeting environmental requirements. Zeolites are highly efficient solid catalysts used in the chemical industry. The design and development of zeolite-based mono-, bi-, and multifunctional catalysts has led to a booming application of zeolite-based catalysts to C1 chemistry. Combining the advantages of zeolites and metallic catalytic species has promoted the catal...

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Isothermal cyclic conversion of methane to methanol using copper-exchanged ZSM-5 zeolite materials under mild conditions

Cited by 16 publications

References 34 publications

Batch Conversion of Methane to Methanol Using Copper Loaded Mordenite: Influence of the Main Variables of the Process

Batch Conversion of Methane to Methanol Using Copper Loaded Mordenite: Influence of the Main Variables of the Process

Methane Utilization to Methanol by a Hybrid Zeolite@Metal–Organic Framework

Applications of Zeolites to C1 Chemistry: Recent Advances, Challenges, and Opportunities

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