Upgrading CO2 to sustainable aromatics via perovskite-mediated tandem catalysis
Guo Tian, Zhengwen Li, Chenxi Zhang, Xinyan Liu, Xiaoyu Fan, Kui Shen, Haibing Meng, Ning Wang, Hao Xiong, Mingyu Zhao, Xiaoyu Liang, Liqiang Luo, Lan Zhang, Binhang Yan, Xiao Chen, Hong‐Jie Peng, Fei Wei
Abstract
Abstract The directional transformation of carbon dioxide (CO 2 ) with renewable hydrogen into specific carbon-heavy products (C 6+ ) of high value presents a sustainable route for net-zero chemical manufacture. However, it is still challenging to simultaneously achieve high activity and selectivity due to the unbalanced CO 2 hydrogenation and C–C coupling rates on complementary active sites in a bifunctional catalyst, thus causing unexpected secondary reaction. Here we report LaFeO 3 perovskite-mediated directional tandem conversion of CO 2 towards heavy aromatics with high CO 2 conversion (> 60%), exceptional aromatics selectivity among hydrocarbons (> 85%), and no obvious deactivation for 1000 hours. This is enabled by disentangling the CO 2 hydrogenation domain from the C-C coupling domain in the tandem system for Iron-based catalyst. Unlike other active Fe oxides showing wide hydrocarbon product distribution due to carbide formation, LaFeO 3 by design is endowed with superior resistance to carburization, therefore inhibiting uncontrolled C–C coupling on oxide and isolating aromatics formation in the zeolite. In-situ spectroscopic evidence and theoretical calculations reveal an oxygenate-rich surface chemistry of LaFeO 3 , that easily escape from the oxide surface for further precise C–C coupling inside zeolites, thus steering CO 2 -HCOOH/H 2 CO-Aromatics reaction pathway to enable a high yield of aromatics.