Insight into Acetic Acid Synthesis from the Reaction of CH<sub>4</sub> and CO<sub>2</sub>

Tu, Chunyan; Nie, Xiaowa; Chen, Jingguang G.

doi:10.1021/acscatal.0c05492

Cited by 62 publications

(52 citation statements)

References 113 publications

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“…270,271 Direct conversion of methane to acetic acid has attracted significant attention due to the wide use of CH 3 COOH as commodity chemicals such as vinyl acetate, acetate esters (ethylene-vinyl acetate, ethyl acetate, etc.). 272 Global CH 3 COOH production was 9.07 million tons in 2020 and is expected to increase up to 11.85 million tons by 2026. 273 Direct acetic acid production from methane oxidation can suppress energetics and the cost of currently used multistep conversion methane to syngas (CO and H 2 ) followed by methanol and acetic acid formation via carbonylation with CO (CH 4 → CO/H 2 → CH 3 OH + CO → 2CH 3 COOH).…”

Section: Characterization Of Sacsmentioning

confidence: 99%

Single Atom Catalysts for Selective Methane Oxidation to Oxygenates

Kumar

Al‐Attas

et al. 2022

ACS Nano

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Direct conversion of methane (CH 4 ) to C 1−2 liquid oxygenates is a captivating approach to lock carbons in transportable value-added chemicals, while reducing global warming. Existing approaches utilizing the transformation of CH 4 to liquid fuel via tandemized steam methane reforming and the Fischer−Tropsch synthesis are energy and capital intensive. Chemocatalytic partial oxidation of methane remains challenging due to the negligible electron affinity, poor C−H bond polarizability, and high activation energy barrier. Transition-metal and stoichiometric catalysts utilizing harsh oxidants and reaction conditions perform poorly with randomized product distribution. Paradoxically, the catalysts which are active enough to break C−H also promote overoxidation, resulting in CO 2 generation and reduced carbon balance. Developing catalysts which can break C−H bonds of methane to selectively make useful chemicals at mild conditions is vital to commercialization. Single atom catalysts (SACs) with specifically coordinated metal centers on active support have displayed intrigued reactivity and selectivity for methane oxidation. SACs can significantly reduce the activation energy due to induced electrostatic polarization of the C−H bond to facilitate the accelerated reaction rate at the low reaction temperature. The distinct metal−support interaction can stabilize the intermediate and prevent the overoxidation of the reaction products. The present review accounts for recent progress in the field of SACs for the selective oxidation of CH 4 to C 1−2 oxygenates. The chemical nature of catalytic sites, effects of metal−support interaction, and stabilization of intermediate species on catalysts to minimize overoxidation are thoroughly discussed with a forward-looking perspective to improve the catalytic performance.

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Section: Characterization Of Sacsmentioning

confidence: 99%

Single Atom Catalysts for Selective Methane Oxidation to Oxygenates

Kumar

Al‐Attas

et al. 2022

ACS Nano

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“…Acetic acid, one of the most important intermediates, has been widely used to produce vinyl acetate monomers, acetic anhydride, and acetic esters. [7] The selective conversion of methane to acetic acid has always attracted significant attention in practical production and academic research. [8] Recently, outstanding progress has been made in acetic acid production through direct methane oxidative carbonylation.…”

Section: Introductionmentioning

confidence: 99%

Highly Selective Carbonylation of CH₃Cl to Acetic Acid Catalyzed by Pyridine‐Treated MOR Zeolite

et al. 2022

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The selective conversion of methane to high value-added chemicals under mild conditions is of great significance for the commercially viable and sustainable utilization of methane but remains a formidable challenge. Herein, we report a strategy for efficiently converting methane to acetic acid via CH 3 Cl as an intermediate. Up to 99.3 % acetic acid and methyl acetate (AA + MA) selectivity was achieved over pyridine-pretreated MOR (MOR-8) under moderate conditions of 523 K and 2.0 MPa. Water, conventionally detrimental to carbonylation reaction over zeolite catalysts, was conducive to the production of AA in the current reaction system. In the 100 h continuous test with the MOR-8 catalyst, the average AA + MA selectivity remained over 98 %. AA was formed by carbonylation of methoxy groups within 8-membered rings of MOR followed by hydrolysis. This strategy provided an approach for highly efficient utilization of methane to oxygenates under mild reaction conditions.

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“…However, leakage issues of the stored CO 2 still hinder widespread applications of CCS technologies . In this regard, CO 2 capture and utilization technologies, converting captured CO 2 into value-added products, such as carbon materials , and chemicals, − are attractive alternatives to mitigate CO 2 emissions.…”

Section: Introductionmentioning

confidence: 99%

Fundamental Aspects of Enhancing Low-Temperature CO₂ Splitting to CO on a Double La₂NiFeO₆ Perovskite

et al. 2021

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This paper addresses the synergistic effect of binary Ni–Fe sites in double La2NiFeO6 perovskite on low-temperature CO2 conversion to CO in the reverse water–gas shift-chemical looping process. Experimental investigations and DFT calculations proved that, for the reduction of perovskite, the Ni-site facilitates the formation of surface oxygen vacancies and the adsorption of hydrogen with agile lattice oxygen mobility. Thus, incorporating Ni can improve the reducibility at low temperature. The Fe-site prevents strong adsorption of the CO2 molecules on the La-site to facilitate its direct dissociation into CO molecules, and thereby CO2 conversion increases with Fe loading. Consequently, La2NiFeO6 can satisfy both high reducibility and CO2 splitting activity by the synergy of binary Ni–Fe sites. It presents an average CO productivity of 2.14 mmol/gcat and a maximum CO production rate of 1.69 mmol/gcat·min at 700 °C, more than 4.7-fold and 10-fold higher than each single LaNiO3 and LaFeO3 perovskites, respectively.

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Insight into Acetic Acid Synthesis from the Reaction of CH₄ and CO₂

Cited by 62 publications

References 113 publications

Single Atom Catalysts for Selective Methane Oxidation to Oxygenates

Single Atom Catalysts for Selective Methane Oxidation to Oxygenates

Highly Selective Carbonylation of CH₃Cl to Acetic Acid Catalyzed by Pyridine‐Treated MOR Zeolite

Fundamental Aspects of Enhancing Low-Temperature CO₂ Splitting to CO on a Double La₂NiFeO₆ Perovskite

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Insight into Acetic Acid Synthesis from the Reaction of CH4 and CO2

Cited by 62 publications

References 113 publications

Single Atom Catalysts for Selective Methane Oxidation to Oxygenates

Single Atom Catalysts for Selective Methane Oxidation to Oxygenates

Highly Selective Carbonylation of CH3Cl to Acetic Acid Catalyzed by Pyridine‐Treated MOR Zeolite

Fundamental Aspects of Enhancing Low-Temperature CO2 Splitting to CO on a Double La2NiFeO6 Perovskite

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Product

Resources

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Insight into Acetic Acid Synthesis from the Reaction of CH₄ and CO₂

Highly Selective Carbonylation of CH₃Cl to Acetic Acid Catalyzed by Pyridine‐Treated MOR Zeolite

Fundamental Aspects of Enhancing Low-Temperature CO₂ Splitting to CO on a Double La₂NiFeO₆ Perovskite