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Selective Hydrogenation of CO2 to Aromatics over Composite Catalyst Comprising NaZnFe and Polyethylene Glycol-Modified HZSM-5 with Intra- and Intercrystalline Mesoporous Structure
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2023-05-31 , DOI: 10.1021/acs.iecr.3c00915 Qisheng Jiang 1 , Guiyao Song 1 , Yangzhou Zhai 1 , Chonghao Chen 1 , Zihao Wang 1 , Huimin Yuan 2 , Zhixiang Zhang 2 , Dianhua Liu 1
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2023-05-31 , DOI: 10.1021/acs.iecr.3c00915 Qisheng Jiang 1 , Guiyao Song 1 , Yangzhou Zhai 1 , Chonghao Chen 1 , Zihao Wang 1 , Huimin Yuan 2 , Zhixiang Zhang 2 , Dianhua Liu 1
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CO2 hydrogenation to aromatics can significantly reduce emissions of the CO2 and provide a complementary route for the production of aromatics. Herein, we report a composite catalyst comprising Na- and Zn-promoted Fe catalyst (NaZnFe) and highly stable hierarchical nanocrystalline HZSM-5 modified by PEG for CO2 hydrogenation to aromatics. The subtle synergy between Na and Zn in NaZnFe promoted the formation and exposure of active iron species and the conversion of CO2 and intermediates. In addition, the PEG modification of HZSM-5 cannot only fabricate intracrystalline mesopores to improve mesoporosity but also provide appropriate acidity, endowing high aromatic selectivity and catalytic stability. Significantly, the high-efficiency diffusion on hierarchical HZSM-5 intensifies the synergistic effect in the catalytic system. The composite catalyst could suppress the total selectivity of CO and CH4 to less than 15% with an aromatic selectivity of up to 63.68% among all hydrocarbons and BTX selectivity in aromatics of up to 56.35% at a CO2 conversion of 42.08%.
中文翻译：
NaZnFe 和具有晶内和晶间介孔结构的聚乙二醇改性 HZSM-5 复合催化剂选择性加氢制芳烃
CO 2加氢制芳烃可显着降低CO 2的排放量，为芳烃生产提供了一条补充途径。在此，我们报道了一种复合催化剂，包含 Na 和 Zn 促进的 Fe 催化剂 (NaZnFe) 和经 PEG 改性的高度稳定的多级纳米晶 HZSM-5，用于 CO 2 加氢制芳烃。NaZnFe中Na和Zn之间微妙的协同作用促进了活性铁物种的形成和暴露以及CO 2的转化和中间体。此外，HZSM-5的PEG修饰不仅可以制造晶内介孔以提高介孔率，还可以提供适当的酸度，赋予高芳烃选择性和催化稳定性。值得注意的是，在多级 HZSM-5 上的高效扩散增强了催化体系中的协同效应。该复合催化剂可将CO和CH 4的总选择性抑制在15%以下，在所有烃类中芳烃选择性高达63.68%，BTX在芳烃中的选择性高达56.35%，CO 2转化率为42.08%。
更新日期：2023-05-31
中文翻译：
NaZnFe 和具有晶内和晶间介孔结构的聚乙二醇改性 HZSM-5 复合催化剂选择性加氢制芳烃
CO 2加氢制芳烃可显着降低CO 2的排放量，为芳烃生产提供了一条补充途径。在此，我们报道了一种复合催化剂，包含 Na 和 Zn 促进的 Fe 催化剂 (NaZnFe) 和经 PEG 改性的高度稳定的多级纳米晶 HZSM-5，用于 CO 2 加氢制芳烃。NaZnFe中Na和Zn之间微妙的协同作用促进了活性铁物种的形成和暴露以及CO 2的转化和中间体。此外，HZSM-5的PEG修饰不仅可以制造晶内介孔以提高介孔率，还可以提供适当的酸度，赋予高芳烃选择性和催化稳定性。值得注意的是，在多级 HZSM-5 上的高效扩散增强了催化体系中的协同效应。该复合催化剂可将CO和CH 4的总选择性抑制在15%以下，在所有烃类中芳烃选择性高达63.68%，BTX在芳烃中的选择性高达56.35%，CO 2转化率为42.08%。
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