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High-entropy-perovskite subnanowires for photoelectrocatalytic coupling of methane to acetic acid.
Nie, Siyang; Wu, Liang; Zhang, Qinghua; Huang, Yunwei; Liu, Qingda; Wang, Xun.
Afiliación
  • Nie S; Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, 100084, China.
  • Wu L; School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China.
  • Zhang Q; Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China.
  • Huang Y; Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, 100084, China.
  • Liu Q; Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, 100084, China. liuqingda@mail.tsinghua.edu.cn.
  • Wang X; Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, 100084, China. wangxun@mail.tsinghua.edu.cn.
Nat Commun ; 15(1): 6669, 2024 Aug 06.
Article en En | MEDLINE | ID: mdl-39107324
ABSTRACT
The incorporation of multiple immiscible metals in high-entropy oxides can create the unconventional coordination environment of catalytic active sites, while the high formation temperature of high-entropy oxides results in bulk materials with low specific surface areas. Here we develop the high-entropy LaMnO3-type perovskite-polyoxometalate subnanowire heterostructures with periodically aligned high-entropy LaMnO3 oxides and polyoxometalate under a significantly reduced temperature of 100 oC, which is much lower than the temperature required by state-of-the-art calcination methods for synthesizing high-entropy oxides. The high-entropy LaMnO3-polyoxometalate subnanowires exhibit excellent catalytic activity for the photoelectrochemical coupling of methane into acetic acid under mild conditions (1 bar, 25 oC), with a high productivity (up to 4.45 mmol g‒1cat h‒1) and selectivity ( > 99%). Due to the electron delocalization at the subnanometer scale, the contiguous active sites of high-entropy LaMnO3 and polyoxometalate in the heterostructure can efficiently activate C - H bonds and stabilize the resulted *COOH intermediates, which benefits the in situ coupling of *CH3 and *COOH into acetic acid.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Reino Unido

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Reino Unido