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

Yu Tang, Yuting Li, Victor Fung, Jiang De-en, Weixin Huang, Shiran Zhang, Yasuhiro Iwasawa, Tomohiro Sakata, Luan Nguyen, Xiaoyan Zhang, Anatoly I. Frenkel and Franklin (Feng) Tao ()
Additional contact information
Yu Tang: University of Kansas
Yuting Li: University of Kansas
Victor Fung: University of California
Jiang De-en: University of California
Weixin Huang: University of Kansas
Shiran Zhang: University of Kansas
Yasuhiro Iwasawa: The University of Electro-Communications
Tomohiro Sakata: The University of Electro-Communications
Luan Nguyen: University of Kansas
Xiaoyan Zhang: University of Kansas
Anatoly I. Frenkel: Stony Brook University
Franklin (Feng) Tao: University of Kansas

Nature Communications, 2018, vol. 9, issue 1, 1-11

Abstract: Abstract Catalytic transformation of CH4 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 CH4 to acetic acid and methanol through coupling of CH4, CO and O2 on single-site Rh1O5 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 Rh1O5 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 CH4 is activated by Rh1O5 anchored on the wall of micropores of ZSM-5; the formed CH3 then couples with CO and OH, to produce acetic acid over a low activation barrier.

Date: 2018
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DOI: 10.1038/s41467-018-03235-7

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