Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions

• Published in: Nature communications Vol. 9; no. 1; pp. 1231 - 11
• Main Authors: Tang, Yu, Li, Yuting, Fung, Victor, Jiang, De-en, Huang, Weixin, Zhang, Shiran, Iwasawa, Yasuhiro, Sakata, Tomohiro, Nguyen, Luan, Zhang, Xiaoyan, Frenkel, Anatoly I., Tao, Franklin (Feng)
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 26.03.2018; Nature Publishing Group; Nature Portfolio
• Subjects: 639/4077/4057; 639/638/77/885; 639/638/77/887; Acetic acid; Acids; Aluminosilicates; Aluminum silicates; carbon capture and storage; Catalysis; catalytic mechanisms; Cations; Chemical industry; Computer applications; Coupling (molecular); heterogeneous catalysis; Humanities and Social Sciences; Hydrogen bonds; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Methane; multidisciplinary; Raw materials; Rhodium; Science; Science (multidisciplinary); Shale; Shale gas; Shales
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-018-03235-7

Catalytic transformation of CH 4 under a mild condition is significant for efficient utilization of shale gas under the circumstance of switching raw materials of chemical industries to shale gas. Here, we report the transformation of CH 4 to acetic acid and methanol through coupling of CH 4 , CO and O 2 on single-site Rh 1 O 5 anchored in microporous aluminosilicates in solution at ≤150 °C. The activity of these singly dispersed precious metal sites for production of organic oxygenates can reach about 0.10 acetic acid molecules on a Rh 1 O 5 site per second at 150 °C with a selectivity of ~70% for production of acetic acid. It is higher than the activity of free Rh cations by >1000 times. Computational studies suggest that the first C–H bond of CH 4 is activated by Rh 1 O 5 anchored on the wall of micropores of ZSM-5; the formed CH 3 then couples with CO and OH, to produce acetic acid over a low activation barrier. Catalytic transformation of CH 4 under mild conditions has implications to shale gas utilization. Here, the authors report the transformation of CH 4 to acetic acid through coupling of CH 4 , CO and O 2 on single-site Rh 1 O 5 anchored in microporous aluminosilicates in liquid phase.