Your browser doesn't support javascript.
loading
Directional Shunting of Photogenerated Carriers in POM@MOF for Promoting Nitrogen Adsorption and Oxidation.
Li, Xiaohong; Yang, Lan; Liu, Qilong; Bai, Wei; Li, Huiyi; Wang, Mengxiang; Qian, Qizhu; Yang, Qinghua; Xiao, Chong; Xie, Yi.
Afiliación
  • Li X; Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
  • Yang L; Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
  • Liu Q; Institute of Energy, Hefei Comprehensive National Science Center, Hefei, Anhui, 230031, P. R. China.
  • Bai W; Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
  • Li H; Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
  • Wang M; Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
  • Qian Q; Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
  • Yang Q; Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
  • Xiao C; Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
  • Xie Y; Institute of Energy, Hefei Comprehensive National Science Center, Hefei, Anhui, 230031, P. R. China.
Adv Mater ; 35(44): e2304532, 2023 Nov.
Article en En | MEDLINE | ID: mdl-37595959
The efficient catalysis of nitrogen (N2 ) into high-value N-containing products plays a crucial role in the N economic cycle. However, weak N2 adsorption and invalid N2 activation remain two major bottlenecks in rate-determining steps, leading to low N2 fixation performance. Herein, an effective dual active sites photocatalyst of polyoxometalates (POMs)-based metal-organic frameworks (MOFs) is highlighted via altering coordination microenvironment and inducing directional shunting of photogenerated carriers to facilitate N2 /catalyst interaction and enhance oxidation performance. MOFs create more open unsaturated metal cluster sites with unoccupied d orbital possessing Lewis acidity to accept electrons from the 3σg bonding orbital of N2 for storage by combining with POMs to replace bidentate linkers. POMs act as electron sponges donating electrons to MOFs, while the holes directional flow to POMs. The hole-rich POMs with strong oxidation capacity are easily involved in oxidizing adsorbed N2 . Taking UiO-66 (C48 H28 O32 Zr6 ) and Mo72 Fe30 ([Mo72 Fe30 O252 (CH3 COO)12 {Mo2 O7 (H2 O)}2 {H2 Mo2 O8 (H2 O)}(H2 O)91 ]·150H2 O) as an example, Mo72 Fe30 @UiO-66 shows twofold enhanced adsorption of N2 (250.5 cm3  g-1 ) than UiO-66 (122.9 cm3 g-1 ) at P/P0  = 1. And, the HNO3 yield of Mo72 Fe30 @UiO-66 is 702.4 µg g-1  h-1 , ≈7 times and 24 times higher than UiO-66 and Mo72 Fe30 . This work provides reliable value for the storage and relaying artificial N2 fixation.
Palabras clave
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Adv Mater Asunto de la revista: BIOFISICA / QUIMICA Año: 2023 Tipo del documento: Article Pais de publicación: Alemania
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Adv Mater Asunto de la revista: BIOFISICA / QUIMICA Año: 2023 Tipo del documento: Article Pais de publicación: Alemania