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Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions
Tang, Yu Li, Yuting Fung, Victor Jiang, De-en Huang, Weixin Zhang, Shiran Iwasawa, Yasuhiro Sakata, Tomohiro Nguyen, Luan Zhang, Xiaoyan
Tang, Yu
Li, Yuting
Fung, Victor
Jiang, De-en
Huang, Weixin
Zhang, Shiran
Iwasawa, Yasuhiro
Sakata, Tomohiro
Nguyen, Luan
Zhang, Xiaoyan
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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.
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2018-03-26
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Nature Publishing Group
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Tang, Y., Li, Y., Fung, V., Jiang, D., Huang, W., Zhang, S., … Tao, F. (Feng). (2018). Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions. Nature Communications, 9, 1231. http://doi.org/10.1038/s41467-018-03235-7