Lewis acid (Ni2+, Co2+/3+or Zn2+) modified electron-deficient Ir4+in IrO2/CuO for promoting methane oxidation to ethanol and methanol

This work delineates the first attempt to tune the product distribution between methanol and ethanol in the direct oxidation of methane reaction by incorporating Lewis acids Ni2+, Co2+/3+or Zn2+into IrO2/CuO. The electrophilicity of Ir4+and the (LAS-BAS)/LAS ratio (LAS: Lewis acid sites, BAS: Brønsted acid sites) are demonstrated to be two reactivity descriptors motivating CH4activation and ethanol formation, respectively. Electron-deficient Ir4+motivates enriched *CH3concentration and subsequent C-C coupling for C2H4formation, while the Lewis acid promotes ethanol formation from C2H4involving lattice O and H2O. The ethanol selectivity presents a quasi-linear relationship with (LAS-BAS)/LAS. © The Royal Society of Chemistry 2021.

Authors
Yang L. 1 , Huang J. 1 , Cen J.2 , Chen D.-L.2 , Zeng H.1 , Rui Z.1 , Luque R. 3, 4 , Duan P.5
Journal
Journal of Materials Chemistry A
Publisher
Royal Society of Chemistry
Number of issue
11
Language
English
Pages
7094-7101
Status
Published
Link
External link
DOI
10.1039/d0ta10842a
Volume
9
Year
2021
Organizations
  • 1 School of Chemical Engineering and Technology, Guangdong Engineering Technology Research Center for Platform Chemicals from Marine Biomass and Their Functionalization, Sun Yat-sen University, Zhuhai, 519082, China
  • 2 Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua, 321004, China
  • 3 Departamento de Química Orgánica, Universidad de Córdoba, Campus de Rabanales, Edificio Marie Curie (C-3), Ctra Nnal IV-A, Km 396, Cordoba, E14014, Spain
  • 4 Peoples Friendship University of Russia (RUDN University), 6 Miklukho-Maklaya Str., Moscow, 117198, Russian Federation
  • 5 Shaanxi Key Laboratory of Energy Chemical Process Intensification, School of Chemical Engineering and Technology, Xi'an Jiaotong University, No. 28, West Xianning Road, Xi'an, Shaanxi 710049, China
Keywords
Ethanol; Methane; Methanol; Direct oxidation; Electron-deficient; Electrophilicity; Ethanol formation; Methane oxidation; Product distributions; Quasi-linear relationship; Reactivity descriptors; Iridium compounds
Date of creation
20.04.2021
Date of change
20.04.2021
Short link
https://repository.rudn.ru/en/records/article/record/72020/
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