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Mechanistic Insights into the Direct Deoxygenation of Phenolic Compounds over Novel Heusler Alloy Catalysts.
Wu, Zewen; Ma, Shenggui; Weng, Shuxian; Liu, Hongying; Jin, Ziheng; Jiang, Xia.
Afiliación
  • Wu Z; College of Architecture and Environment, Sichuan University, Chengdu 610065, China.
  • Ma S; College of Carbon Neutrality Future Technology, Sichuan University, Chengdu 610065, China.
  • Weng S; College of Carbon Neutrality Future Technology, Sichuan University, Chengdu 610065, China.
  • Liu H; Tianfu Yongxing Laboratory, Chengdu 610213, China.
  • Jin Z; Tianfu Yongxing Laboratory, Chengdu 610213, China.
  • Jiang X; Tianfu Yongxing Laboratory, Chengdu 610213, China.
ACS Appl Mater Interfaces ; 16(29): 38111-38123, 2024 Jul 24.
Article en En | MEDLINE | ID: mdl-39007495
ABSTRACT
The catalytic deoxygenation of phenolic compounds is a crucial step in the valorization of biomass resources, which can effectively enhance the heating value and stability of primary biofuel. In this study, the catalytic mechanism of four Heusler alloy catalysts for the direct deoxidation pathway of phenol was studied through electronic structure regulation by element occupation. We found that Heusler alloys catalysts exhibit excellent catalytic activity in the dissociation activation of H2 and the cleavage of aryl hydroxyl bond (CAr-OH) bonds. The energy barriers for the direct cleavage of the CAr-OH bond in phenol on Ni2MoAl, Co2MoAl, Ni2NbAl and Ni2MoGa catalysts are 0.86, 0.95, 1.09, and 1.28 eV, respectively. And Y element of the X2YZ catalyst has a significant impact on this reaction, while the X element has a complex influence on the hydrogenation step of the unsaturated benzene ring. Microkinetic analysis further substantiates that the phenol (CAr-OH) bond cleavage step in the reaction exhibits a fast reaction rate and high extent of reaction. The reaction of hydroxyl hydrogenation to produce water exhibits the highest energy barrier, serving as the rate-determining step of the entire reaction. This issue could potentially be addressed by further fine-tuning the electronic structure.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: ACS Appl Mater Interfaces Asunto de la revista: BIOTECNOLOGIA / ENGENHARIA BIOMEDICA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Estados Unidos

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: ACS Appl Mater Interfaces Asunto de la revista: BIOTECNOLOGIA / ENGENHARIA BIOMEDICA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Estados Unidos