The production of acetone through ketonization of acetic acid is both energy intensive and environmentally 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.

中文翻译：

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活性位点集成了使丙酮产生的CO ₂和CH ₄的CC耦合

通过乙酸酮化生产丙酮既耗能又对环境有害，因为它释放出等分子的CO ₂。在此，基于广泛的密度泛函理论计算研究，通过连续的C–C偶联，提出了一种由CO ₂和CH ₄产生丙酮的新方法。为了实现连续的C-C偶联，构建了掺杂有Zn原子团的CeO ₂基催化剂。CH ₃ *与乙酸盐物质的直接偶联，是由CO ₂和稳定的CH _3的C–C偶联形成的*，可以实现生产丙酮。结果表明，在基于CeO ₂的催化剂上构建的活性位点集合体上，碳链的生长是可能的。乙酸酯物质与甲基部分的偶联遵循亲核加成机理，并且在O _vac（氧空位）和中性表面上分别具有0.25和0.14 eV的表观活化能。该方法有可能取代基于乙酸酮化的传统丙酮生产技术。