Photocatalytic Conversion of Methane: Recent Advancements and Prospects

Li, Qi; Ouyang, Yuxing; Li, Hongliang; Wang, Liangbing; Zeng, Jie

doi:10.1002/anie.202108069

Cited by 152 publications

(92 citation statements)

References 147 publications

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“…Meanwhile, high atom utilization efficiency could be achieved 46 , 47 . On the other hand, since CH 4 exhibited low electron and proton affinity, moderate decoration of defective sites could enhance the chemical-adsorption of non-polar molecular, then promoting the activation of CH 4 48 . Therefore, the integration of both defects and single atom cocatalyst decoration could boost charge separation, weaken oxidative potential and enhance CH 4 activation on a photocatalyst.…”

Section: Introductionmentioning

confidence: 99%

Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light

et al. 2022

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Methane (CH4) oxidation to high value chemicals under mild conditions through photocatalysis is a sustainable and appealing pathway, nevertheless confronting the critical issues regarding both conversion and selectivity. Herein, under visible irradiation (420 nm), the synergy of palladium (Pd) atom cocatalyst and oxygen vacancies (OVs) on In2O3 nanorods enables superior photocatalytic CH4 activation by O2. The optimized catalyst reaches ca. 100 μmol h−1 of C1 oxygenates, with a selectivity of primary products (CH3OH and CH3OOH) up to 82.5%. Mechanism investigation elucidates that such superior photocatalysis is induced by the dedicated function of Pd single atoms and oxygen vacancies on boosting hole and electron transfer, respectively. O2 is proven to be the only oxygen source for CH3OH production, while H2O acts as the promoter for efficient CH4 activation through ·OH production and facilitates product desorption as indicated by DFT modeling. This work thus provides new understandings on simultaneous regulation of both activity and selectivity by the synergy of single atom cocatalysts and oxygen vacancies.

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Section: Introductionmentioning

confidence: 99%

Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light

et al. 2022

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“…•OH is oxidative and has an oxidation potential of 2.8 V (vs. NHE), possibly reacts with CH 4 to afford •CH 3 radical and H 2 O, and the enthalpy variation is about –60 kJ·mol −1 . [ 37 ] In photocatalytic DCCM, •OH can be formed by water, oxygen or hydrogen peroxide.…”

Section: Catalytic Mechanism Of Methane Couplingmentioning

confidence: 99%

Advances and Challenges of Photocatalytic Methane C—C Coupling

2022

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Comprehensive Summary Methane, the main component of natural gas and shale gas, can be converted to upgraded fuels, syngas and value‐added chemicals. Due to the nonpolar character of methane and large bond dissociation energy of sp3 C—H bond, methane conversion requires strong oxidants or acids/bases for its activation. Photocatalysis capable of inducing highly oxidative surrogates enables methane C—H bond scission at room temperature, thereby avoiding side reactions and coke formation caused by high reaction temperature. The scission of methane C—H bond generates •CH3 that may undergo C—C bond coupling with carbon radicals, which is a versatile way to obtain C2+ chemicals. Apart from the kinetically slow activation of methane C—H bond, photocatalysis also suffers from complex product distributions owing to the presence of varieties of radicals during photocatalytic methane conversion, and a low selectivity of desired C2+ products was achieved. In this review, we summarize the recent advances of photocatalytic methane conversion with emphasis on methane C—C bond coupling. Methods of methane C—H bond activation and radical manipulation for selective C—C bond coupling were discussed in detail. We hope this review may be a valuable guide of future work in photocatalytic methane C—C coupling.

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“…Therefore, water oxidation is thermodynamically limited at the n-Si photoelectrode under methane oxidation conditions. Lastly, other materials such as metal chalcogenide, carbonderived materials, C 3 N 4 , metal carbide can be candidates for PEC methane oxidation because these materials have been reported to show the photocatalytic activity for partial oxidation of methane in the PC system [2].…”

Section: Potential Semiconductor Materialsmentioning

confidence: 99%

“…Methane is a major ingredient in biogas, natural gas, coal-bed gas, shale gas, and gas hydrates. In addition to conventional natural gas, unconventional natural gas, including shale gas, coal-bed gas, and tight gas, have also recently attracted much attention for methane extraction, because of their abundance [1,2]. Since methane has the highest H/C ratio and heat of combustion among hydrocarbons, it is utilized as a fuel for transportation and heating, and for industrial uses.…”

Section: Introductionmentioning

confidence: 99%

Photoelectrochemical Conversion of Methane into Value-Added Products

2021

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Methane has been reported to be directly converted into value-added products through various methods. Among them, photoelectrochemical (PEC) methane conversion is considered an eco-friendly method because it utilizes solar light and is able to control the selectivity to different products by means of application of an external bias. Recently, some PEC methane conversion systems have been reported, but their performance efficiencies are relatively lower than those of other existing thermal, photocatalytic, and electrochemical systems. The detailed mechanism of methane activation is not clear at this stage. In this review, various catalytic materials and their roles in the reaction pathways are summarized and discussed. Furthermore, promising semiconductor materials, co-catalysts, and oxidants have also been proposed. Finally, direct and indirect pathways in the design of the PEC methane conversion system have been discussed.

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Photocatalytic Conversion of Methane: Recent Advancements and Prospects

Cited by 152 publications

References 147 publications

Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light

Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light

Advances and Challenges of Photocatalytic Methane C—C Coupling

Photoelectrochemical Conversion of Methane into Value-Added Products

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