Direct Photocatalytic Synthesis of Acetic Acid from Methane and CO at Ambient Temperature Using Water as Oxidant

Dong, Chunyang; Marinova, Maya; Tayeb, K. Ben; Safonova, Оlga V.; Zhou, Yong; Hu, Di; Chernyak, S. A.; Corda, Massimo; Zaffran, Jérémie; Khodakov, Andreï Y.

doi:10.1021/jacs.2c10840

Cited by 38 publications

(36 citation statements)

References 55 publications

(73 reference statements)

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“…The peak observed at 2104 cm −1 is attributed to the absorbed *CO, which is regarded as a key intermediate for C 2+ products. 40 Also, we deduced that the *CO adsorbed on N sub promoted *CO coupling with *CH 3 to form C 2+ products.…”

Section: T H Imentioning

confidence: 85%

Nitrogen-Doped Titanium Dioxide for Selective Photocatalytic Oxidation of Methane to Oxygenates

Feng,

Mao,

Sun

et al. 2024

ACS Appl. Mater. Interfaces

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Photocatalytic conversion of methane (CH 4 ) to value-added chemicals using H 2 O as the oxidant under mild conditions is a desired sustainable pathway for synthesizing commodity chemicals. However, controlling product selectivity while maintaining high product yields is greatly challenging. Herein, we develop a highly efficient strategy, based on the precise control of the types of nitrogen dopants, and the design of photocatalysts, to achieve high selectivity and productivity of oxygenates via CH 4 photocatalytic conversion. The primary product (methanol) is obtained in a high yield of 159.8 μmol•g −1 •h −1 and 47.7% selectivity, and the selectivity of oxygenate compounds reached 92.5%. The unique hollow porous structure and substituted nitrogen sites of nitrogen-doped TiO 2 synergistically promote its photo-oxidation performance. Furthermore, in situ attenuated total reflectance Fourier transform infrared spectroscopy provides direct evidence of the key intermediates and their evolution for producing methanol and multicarbon oxygenates. This study provides insights into the mechanism of photocatalytic CH 4 conversion.

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Section: T H Imentioning

confidence: 85%

Nitrogen-Doped Titanium Dioxide for Selective Photocatalytic Oxidation of Methane to Oxygenates

Feng,

Mao,

Sun

et al. 2024

ACS Appl. Mater. Interfaces

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“…Asymmetric coupling between alkyls and carbon monoxide ( * CH x ─ * CO) is initiated on the anode because this is energetically and kinetically favorable. [28,29] The coupling between * CH 3 and * CO occurs (early) during the formation of C 2+ products [30,31] where methylcarbonyl species ( * COCH 3 ) are critical intermediates. Additionally, * COCH 3 can be generated from the OH ads -assisted oxidation of * C 2 H 5 , Figure 4c, Pathway iv.…”

Section: Mechanistic View Of Tandem Plasma-electrocatalysismentioning

confidence: 99%

Mild Methane Electrochemical Oxidation Boosted via Plasma Pre‐Activation

Sun

Wang

Davey

et al. 2023

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Obtaining partial methane oxidation reaction (MOR) with various oxygenates via a mild electrochemical method is practically difficult because of activation of stable C─H bond and consequent reaction pathway regulation. Here, a real‐time tandem MOR with cascaded plasma and electrocatalysis to activate and convert the methane (CH4) synergistically is reported for the first time. Boosted CH4 conversion is demonstrated toward value‐added products including, alcohols, carboxylates, and ketone via use of commercial Pd‐based electrocatalysts. Compared with hash industrial processes, a mild condition, that is, anode potential < 1.0 V versus RHE (reversible hydrogen electrode) is used that mitigates overoxidation of oxygenates and obviates competing reaction(s). One evidence that Pd(II) sites and surface adsorbed hydroxyls are important in facilitating activated‐CH4 species conversion, and establish a reaction mechanism for conversion(s) that involves coupling reactions between adsorbed hydroxyls, carbon monoxide and C1/C2 alkyls. One conclude that pre‐activation is important in boosting electrochemical partial MOR under mild conditions and will be of benefit in the development of sustainable CH4 conversion technology.

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“…Most studies on the photocatalytic synthesis of methanol from CH 4 and H 2 O have focused on the use of ultraviolet light or stronger lasers to excite WO 3 and BiVO 4 ‐based catalysts, but low conversion rates still remain challenging. Recently, Ordomsky's group, [ 90 ] reported a new photocatalytic reaction pathway, through which CH 3 COOH could be directly synthesized from CH 4 , CO, and H 2 O over Pt/polyoxometalate/TiO 2 at ambient temperature. Under the optimum conditions, 5.7 mmol L −1 CH 3 COOH could be produced within 60 h with over 90% selectivity.…”

Section: Methane Conversion Driven By Sustainable Energymentioning

confidence: 99%

Sustainable Energy Resources for Driving Methane Conversion

Chen

Weng

2023

Advanced Energy Materials

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The conversion of methane to value‐added chemicals by traditional reforming processes suffers from intensive energy consumption due to its particularly strong C─H bonds. Thus, it is urgent to optimize the driving force structure for methane conversion by accelerating the integration of sustainable energy. In this review, the advances in sustainable energy‐driven methane conversion are systematically summarized to provide a scientific understanding of methane conversion in operation/storage concepts, reactor design, technological maturity, system optimization, and remaining issues. Furthermore, the essence, economic evaluations, energy balance, and social impacts of methane conversion driven by sustainable energy are carefully discussed, paving a path for the future course of research and development. Diversifying the energy mix can play an important role in the future of sustainable energy‐driven methane conversion industries, being used as a crucial step for the transition to sustainable energy, especially the combination of solar/nuclear energy with fossil fuels to produce value‐added chemicals. Additionally, this review intends to bridge the studies of methane conversion and sustainable energy‐driven development, with the ultimate goal of offering a robust framework to understand the current status of sustainable energy‐driven methane conversion and provide guidance for the design of sustainable solutions for a greener future.

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Direct Photocatalytic Synthesis of Acetic Acid from Methane and CO at Ambient Temperature Using Water as Oxidant

Cited by 38 publications

References 55 publications

Nitrogen-Doped Titanium Dioxide for Selective Photocatalytic Oxidation of Methane to Oxygenates

Nitrogen-Doped Titanium Dioxide for Selective Photocatalytic Oxidation of Methane to Oxygenates

Mild Methane Electrochemical Oxidation Boosted via Plasma Pre‐Activation

Sustainable Energy Resources for Driving Methane Conversion

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