Статья

Upgrading CO2 to sustainable aromatics via perovskite-mediated tandem catalysis

Guo TianBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084, Beijing, ChinaZhengwen LiBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084, Beijing, ChinaChenxi ZhangBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084, Beijing, China. [email protected]Xinyan LiuInstitute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, 611731, Sichuan, ChinaXiaoyu FanBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084, Beijing, ChinaKui ShenKey Laboratory of Fuel Cell Technology of Guangdong Province, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640, ChinaHaibing MengCollege of Chemistry, Taiyuan University of Technology, Taiyuan, 030024, ChinaNing WangFaculty of Environment and Life, Beijing University of Technology, 100124, Beijing, ChinaHao XiongBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084, Beijing, ChinaMingyu ZhaoBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084, Beijing, ChinaXiaoyu LiangBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084, Beijing, ChinaLiqiang LuoBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084, Beijing, ChinaLan ZhangFaculty of Environment and Life, Beijing University of Technology, 100124, Beijing, ChinaBinhang YanBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084, Beijing, ChinaXiao ChenBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084, Beijing, China. [email protected]Hong‐Jie PengInstitute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, 611731, Sichuan, China. [email protected]Fei WeiBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084, Beijing, China. [email protected]

2024en

ABI

Аннотация

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.

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Идентификаторы

DOI: 10.1038/s41467-024-47270-z

Цитирования и источники

Цитирований: 2Использованных источников: 0

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