Coupling of electrocatalytic CO<sub>2</sub> reduction and CH<sub>4</sub> oxidation for efficient methyl formate electrosynthesis

Zhang, Quan; Chen, Yangshen; Yan, Shuai; Lv, Ximeng; Yang, Chao; Kuang, Min; Zheng, Gengfeng

doi:10.1039/d4ee00087k

Energy Environ. Sci.

2024

DOI: 10.1039/d4ee00087k

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Coupling of electrocatalytic CO₂ reduction and CH₄ oxidation for efficient methyl formate electrosynthesis

Quan Zhang,

Yangshen Chen,

Shuai Yan

et al.

Abstract: The electrocatalytic carbon dioxide reduction reaction (CO2RR) is promising for converting this greenhouse gas into value-added chemicals, while it suffers from limited energy efficiency and product variability. The direct coupling...

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Cited by 9 publications

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Efficient Photocatalytic CH₄‐to‐Ethanol Conversion by Limiting Interfacial Hydroxyl Radicals Using Gold Nanoparticles

Zhang,

Yang,

Chen

et al. 2024

Angewandte Chemie

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Photocatalytic CH4 oxidation to ethanol with high selectivity is attractive but substantially challenging. The activation of inert C–H bonds at ambient conditions requires highly reactive oxygen species like hydroxyl radicals (·OH), while the presence of those oxidative species also facilitates fast formation of C1 products, instead of the kinetically sluggish C–C coupling to produce ethanol. Herein, we developed a BiVO4 photocatalyst with surface functionalization of Au nanoparticles (BiVO4@Au), which not only enables photogeneration of ·OH to activate CH4 into ·CH3, but also in‐situ consumes those ·OH species to retard their further attack on ·CH3, resulting in an enhanced ·CH3/·OH ratio and facilitating C–C coupling toward ethanol. The ·CH3/·OH ratio is further improved by transporting CH4 via a gas‐diffusion layer to the photocatalytic interface, leading to even higher ethanol selectivity and production rates. At ambient conditions and without photosensitizers or sacrificial agents, the BiVO4@Au photocatalyst exhibited an outstanding CH4‐to‐ethanol conversion performance, including a peak ethanol yield of 680 μmol·g‐1·h‐1, a high selectivity of 86%, and a stable photoconversion of > 100 h, substantially exceeding most of the previous reports. Our work suggests an attractive approach of in‐situ generation and modulation of the ·OH levels for photocatalytic CH4 conversion toward multi‐carbon products.

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Efficient Photocatalytic CH₄‐to‐Ethanol Conversion by Limiting Interfacial Hydroxyl Radicals Using Gold Nanoparticles

Zhang,

Yang,

Chen

et al. 2024

Angewandte Chemie

View full text Add to dashboard Cite

show abstract

Efficient Photocatalytic CH₄‐to‐Ethanol Conversion by Limiting Interfacial Hydroxyl Radicals Using Gold Nanoparticles

Zhang,

Yang,

Chen

et al. 2024

Angew Chem Int Ed

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Anode engineering for electrocatalytic CO2 reduction reaction

Zhang,

Xu,

Yin

et al. 2024

Chinese Chemical Letters

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Coupling of electrocatalytic CO₂ reduction and CH₄ oxidation for efficient methyl formate electrosynthesis

Abstract: The electrocatalytic carbon dioxide reduction reaction (CO2RR) is promising for converting this greenhouse gas into value-added chemicals, while it suffers from limited energy efficiency and product variability. The direct coupling...

Cited by 9 publications

References 30 publications

Efficient Photocatalytic CH₄‐to‐Ethanol Conversion by Limiting Interfacial Hydroxyl Radicals Using Gold Nanoparticles

Efficient Photocatalytic CH₄‐to‐Ethanol Conversion by Limiting Interfacial Hydroxyl Radicals Using Gold Nanoparticles

Efficient Photocatalytic CH₄‐to‐Ethanol Conversion by Limiting Interfacial Hydroxyl Radicals Using Gold Nanoparticles

Anode engineering for electrocatalytic CO2 reduction reaction

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Product

Resources

About

Coupling of electrocatalytic CO2 reduction and CH4 oxidation for efficient methyl formate electrosynthesis

Abstract: The electrocatalytic carbon dioxide reduction reaction (CO2RR) is promising for converting this greenhouse gas into value-added chemicals, while it suffers from limited energy efficiency and product variability. The direct coupling...

Cited by 9 publications

References 30 publications

Efficient Photocatalytic CH4‐to‐Ethanol Conversion by Limiting Interfacial Hydroxyl Radicals Using Gold Nanoparticles

Efficient Photocatalytic CH4‐to‐Ethanol Conversion by Limiting Interfacial Hydroxyl Radicals Using Gold Nanoparticles

Efficient Photocatalytic CH4‐to‐Ethanol Conversion by Limiting Interfacial Hydroxyl Radicals Using Gold Nanoparticles

Anode engineering for electrocatalytic CO2 reduction reaction

Contact Info

Product

Resources

About

Coupling of electrocatalytic CO₂ reduction and CH₄ oxidation for efficient methyl formate electrosynthesis

Efficient Photocatalytic CH₄‐to‐Ethanol Conversion by Limiting Interfacial Hydroxyl Radicals Using Gold Nanoparticles

Efficient Photocatalytic CH₄‐to‐Ethanol Conversion by Limiting Interfacial Hydroxyl Radicals Using Gold Nanoparticles

Efficient Photocatalytic CH₄‐to‐Ethanol Conversion by Limiting Interfacial Hydroxyl Radicals Using Gold Nanoparticles