Chem Catalysis ( IF 11.5 ) Pub Date : 2023-07-05 , DOI: 10.1016/j.checat.2023.100689 Xudong Fang , Bin Li , Hongchao Liu , Mingguan Xie , Zhiyang Chen , Leilei Yang , Jingfeng Han , Wenliang Zhu , Zhongmin Liu
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.
中文翻译:
在酸性沸石催化剂上用氯甲烷将二氧化碳转化为芳烃的高碳利用率
二氧化碳(CO 2 )和甲烷(CH 4 )是主要的温室气体,利用这些C1资源生产高价值化学品对于可持续化学具有重要意义。由于高稳定性和C-C耦合势垒,同时将CO 2和CH 4转化为芳烃仍然具有挑战性。在此,我们报告了一种基于 CO 2和 CH 3 Cl(CH 4的替代品)转化的可持续利用温室气体的策略,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% BTX 选择性。原位表征和13C同位素标记实验表明CO 2通过内酯直接参与芳烃的形成,而不是经历经典的逆水煤气变换反应。此外,提出了一种独特的CO 2转化机制,涉及内酯和环戊烯酮物质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。