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Atomically Dispersed Nickel Anchored on a Nitrogen-Doped Carbon/TiO2 Composite for Efficient and Selective Photocatalytic CH4 Oxidation to Oxygenates.
Song, Hui; Huang, Hengming; Meng, Xianguang; Wang, Qi; Hu, Huilin; Wang, Shengyao; Zhang, Hongwei; Jewasuwan, Wipakorn; Fukata, Naoki; Feng, Ningdong; Ye, Jinhua.
Afiliación
  • Song H; International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.
  • Huang H; International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.
  • Meng X; State Key Laboratory of Materials-Oriented Chemical Engineering, College of Materials Science and Engineering, Nanjing Tech University, Nanjing, 210009, P. R. China.
  • Wang Q; Hebei Provincial Laboratory of Inorganic Nonmetallic Materials, College of Materials Science and Engineering, North China University of Science and Technology, Tangshan, 063210, P. R. China.
  • Hu H; International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.
  • Wang S; Graduate School of Chemical Sciences and Engineering, Hokkaido University, Sapporo, 060-0814, Japan.
  • Zhang H; TJU-NIMS International Collaboration Laboratory, School of Material Science and Engineering, Tianjin University, Tianjin, 300072, P. R. China.
  • Jewasuwan W; College of Science, Huazhong Agricultural University, Wuhan, 430070, P. R. China.
  • Fukata N; Biogas Institute of Ministry of Agriculture and Rural Affairs, Chengdu, 610041, P. R. China.
  • Feng N; International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.
  • Ye J; International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.
Angew Chem Int Ed Engl ; 62(4): e202215057, 2023 Jan 23.
Article en En | MEDLINE | ID: mdl-36446740
Direct photocatalytic oxidation of methane to liquid oxygenated products is a sustainable strategy for methane valorization at room temperature. However, in this reaction, noble metals are generally needed to function as cocatalysts for obtaining adequate activity and selectivity. Here, we report atomically dispersed nickel anchored on a nitrogen-doped carbon/TiO2 composite (Ni-NC/TiO2 ) as a highly active and selective catalyst for photooxidation of CH4 to C1 oxygenates with O2 as the only oxidant. Ni-NC/TiO2 exhibits a yield of C1 oxygenates of 198 µmol for 4 h with a selectivity of 93 %, exceeding that of most reported high-performance photocatalysts. Experimental and theoretical investigations suggest that the single-atom Ni-NC sites not only enhance the transfer of photogenerated electrons from TiO2 to isolated Ni atoms but also dominantly facilitate the activation of O2 to form the key intermediate ⋅OOH radicals, which synergistically lead to a substantial enhancement in both activity and selectivity.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2023 Tipo del documento: Article País de afiliación: Japón Pais de publicación: Alemania

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2023 Tipo del documento: Article País de afiliación: Japón Pais de publicación: Alemania