Active Site Ensembles Enabled C-C Coupling of CO2 and CH4 for Acetone Production

作者：Zhao, Yuntao; Wang, Hua; Han, Jinyu; Zhu, Xinli^*; Ge, Qingfeng^*

来源：Journal of Physical Chemistry C, 2018, 122(17): 9570-9577.

DOI：10.1021/acs.jpcc.8b02359

• AUGMENTED-WAVE METHOD
• ACETIC-ACID
• CARBOXYLIC-ACIDS
• CARBON-DIOXIDE
• TRANSITION-METALS
• KETONIZATION
• METHANE
• CONVERSION
• CATALYSTS
• MECHANISM

The production of acetone through ketonization of acetic acid is both energy intensive and environmentally C-C Coupling detrimental, as it emits equimolecular CO2. Herein, a novel approach for acetone production from CO2 and CH4 was proposed through consecutive C-C coupling based on an extensive density functional theory computational study. To realize the consecutive C-C coupling, CeO2-based catalyst doped with Zn site ensemble was constructed. Direct coupling of CH3* with the acetate species, formed from C-C coupling of CO2 and stabilized CH3*, could be achieved to produce acetone. The results show that carbon chain growth is possible on the active site ensembles constructed on a CeO2-based catalyst. The coupling of the acetate species with the methyl moiety follows a nucleophilic addition mechanism and has apparent activation energies of 0.25 and 0.14 eV on O-vac (oxygen vacancy) and neutral surfaces, respectively. This process could potentially replace the traditional acetone production technology based on ketonization of acetic acid.

• 出版日期2018-5-3
• 单位天津大学