Title :

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

Author(s) :

Dong, Chunyang [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Marinova, Maya [Auteur]
Unité Matériaux et Transformations - UMR 8207 [UMET]
Ben Tayeb Meziane, Karima [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516
Safonova, Olga V. [Auteur]
Paul Scherrer Institute [PSI]
Zhou, Yong [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Hu, Di [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Cherniak, Sergei [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Corda, Massimo [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Zaffran, Jeremie [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Khodakov, Andrei [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Ordomsky, Vitaly [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]

Journal title :

Journal of the American Chemical Society

Abbreviated title :

J Am Chem Soc

Volume number :

145

Pages :

1185-1193

Publisher :

American Chemical Society

Publication date :

2023-01-02

ISSN :

1520-5126

English keyword(s) :

Catalysts
Hydrocarbons
Irradiation
Oxides
Platinum

HAL domain(s) :

Chimie/Catalyse
Chimie/Chimie théorique et/ou physique

English abstract : [en]

Direct functionalization of methane selectively to value-added chemicals is still one of the main challenges in modern science. Acetic acid is an important industrial chemical produced nowadays by expensive and environmentally ...
Show more >Direct functionalization of methane selectively to value-added chemicals is still one of the main challenges in modern science. Acetic acid is an important industrial chemical produced nowadays by expensive and environmentally unfriendly carbonylation of methanol using homogeneous catalysts. Here, we report a new photocatalytic reaction route to synthesize acetic acid from CH4 and CO at room temperature using water as the sole external oxygen source. The optimized photocatalyst consists of a TiO2 support and ammonium phosphotungstic polyoxometalate (NPW) clusters anchored with isolated Pt single atoms (Pt1). It enables a stable synthesis of 5.7 mmol·L–1 acetic acid solution in 60 h with the selectivity over 90% and 66% to acetic acid on liquid-phase and carbon basis, respectively, with the production of 99 mol of acetic acid per mol of Pt. Combined isotopic and in situ spectroscopy investigation suggests that synthesis of acetic acid proceeds via a photocatalytic oxidative carbonylation of methane over the Pt1 sites, with the methane activation facilitated by water-derived hydroxyl radicals.Show less >

Language :

Anglais

Audience :

Internationale

Popular science :

Non

Administrative institution(s) :

Université de Lille
CNRS
Centrale Lille
ENSCL
Univ. Artois

Collections :

• Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516
• Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
• Unité Matériaux et Transformations (UMET) - UMR 8207

Research team(s) :

Catalyse pour l’énergie et la synthèse de molécules plateforme (CEMOP)
Propriétés magnéto structurales des matériaux (PMSM)

Submission date :

2023-06-05T08:05:45Z
2023-06-28T09:15:48Z