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Photocatalytic CH4-to-Ethanol Conversion on Asymmetric Multishelled Interfaces.
Hao, Shuya; Xue, Yuanyuan; Peng, Chen; Mi, Yuying; Yan, Yaqin; Wang, Maoyin; Han, Qing; Zheng, Gengfeng.
Afiliación
  • Hao S; Laboratory of Advanced Materials, Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, China.
  • Xue Y; Laboratory of Advanced Materials, Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, China.
  • Peng C; Laboratory of Advanced Materials, Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, China.
  • Mi Y; Laboratory of Advanced Materials, Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, China.
  • Yan Y; Laboratory of Advanced Materials, Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, China.
  • Wang M; Laboratory of Advanced Materials, Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, China.
  • Han Q; Laboratory of Advanced Materials, Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, China.
  • Zheng G; Laboratory of Advanced Materials, Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, China.
J Am Chem Soc ; 146(37): 25870-25877, 2024 Sep 18.
Article en En | MEDLINE | ID: mdl-39231938
ABSTRACT
The selective oxidation of methane (CH4) features attractive potentials in both mitigating global warming and producing value-added chemicals. However, due to the short-life and unpaired concentrations of reactive intermediates (such as ·OH, ·CH3, and CO), the selective formation of multicarbon products like ethanol has remained challenging. In this work, we developed a hollow multishelled CeO2@PdO@FeOx nanosphere catalyst with two asymmetric and closely connected interfaces, featuring efficient in-tandem photo-oxidation of CH4 into ethanol with O2 as the oxidant. The outer FeOx surface promotes the photoreduction of the oxazole atoms in O2. In the meantime, the two asymmetric PdO/FeOx and CeO2/PdO catalytic interfaces enable selective photoactivation of CH4 to ·CH3 and then to CO, respectively, and the hollow multishelled structure further facilitates the directional transport and coupling of the as-generated ·CH3 and CO to produce ethanol. Under 100 mW·cm-2 light intensity and ambient conditions, the hollow multishelled CeO2@PdO@FeOx nanosphere photocatalyst exhibited a peak CH4-to-ethanol yield of 728 µmol·g-1·h-1 without photosensitizers or sacrificial agents, almost three times higher than the previous best reports on photocatalytic CH4 oxidation to ethanol, suggesting the attractive potential of the asymmetric multishelled catalytic interfaces.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
Imprimir
XML
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Estados Unidos