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High carbon utilization for CO2 conversion with chloromethane to aromatics over acidic zeolite catalyst

机译:在酸性沸石催化剂上将氯甲烷转化为芳烃的CO2的高碳利用率

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Carbon dioxide (CO2) and methane (CH4) are major greenhouse gases, and the use of these C1 resources to produce high-value chemicals is significant for sustainable chemistry. Due to the high stability and C-C coupling barriers, simultaneous conversion of CO2 and CH4 to aromatics remains challenging. Herein, we report a sustainable strategy for utilizing greenhouse gases based on the conversion of CO2 and CH3Cl, an alternative of CH4, that yields a high aromatics selectivity (71.3) with -50 BTX selectivity using H-ZSM-5 as catalyst at 723 K and 3 MPa. In situ characterization and 13C isotope-labeling experiments demonstrate that CO2 directly participates in the formation of aromatics via lactone species instead of undergoing a classical reverse water-gas shift reaction. Furthermore, a unique mechanism for CO2 conversion is proposed, involving the formation and subsequent transformation of lactone and cyclopentenone species. This work expands high carbon utilization pathways for converting greenhouse gases into chemicals.
机译:二氧化碳 (CO2) 和甲烷 (CH4) 是主要的温室气体,利用这些 C1 资源生产高价值化学品对可持续化学具有重要意义。由于高稳定性和 C-C 偶联势垒,将 CO2 和 CH4 同时转化为芳烃仍然具有挑战性。在此,我们报告了一种基于CO2和CH3Cl(CH4的替代品)转化的可持续温室气体利用策略,该策略使用H-ZSM-5作为催化剂,在723 K和3 MPa下产生高芳烃选择性(71.3%)和-50%的BTX选择性。原位表征和13C同位素标记实验表明,CO2通过内酯种类直接参与芳烃的形成,而不是经历经典的逆水-气变换反应。此外,还提出了一种独特的CO2转化机制,涉及内酯和环戊烯酮物种的形成和随后的转化。这项工作扩展了将温室气体转化为化学品的高碳利用途径。

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