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- Title
Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions.
- Authors
Yu Tang; Yuting Li; Victor Fung; De-en Jiang; Weixin Huang; Shiran Zhang; Yasuhiro Iwasawa; Tomohiro Sakata; Luan Nguyen; Xiaoyan Zhang; Frenkel, Anatoly I.; Franklin (Feng) Tao
- 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.
- Subjects
RHODIUM; ACETIC acid; SHALE gas industry; CHEMICAL industry; SHALE gas; METHANE as fuel
- Publication
Nature Communications, 2018, Vol 9, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-018-03235-7