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.

Details

Title
Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions
Author
Tang, Yu 1   VIAFID ORCID Logo  ; Li, Yuting 1 ; Fung, Victor 2 ; De-en, Jiang 2   VIAFID ORCID Logo  ; Huang, Weixin 3 ; Zhang, Shiran 3 ; Iwasawa, Yasuhiro 4 ; Sakata, Tomohiro 4 ; Nguyen, Luan 3 ; Zhang, Xiaoyan 5 ; Frenkel, Anatoly I 6 ; Franklin (Feng) Tao 3   VIAFID ORCID Logo 

1  Department of Chemical and Petroleum Engineering and Department of Chemistry, University of Kansas, Lawrence, KS, USA 
2  Department of Chemistry, University of California, Riverside, CA, USA 
3  Department of Chemical and Petroleum Engineering and Department of Chemistry, University of Kansas, Lawrence, KS, USA; Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, IN, USA 
4  Innovation Research Center for Fuel Cells and Graduate School of Informatics and Engineering, The University of Electro-Communications, Chofu, Tokyo, Japan 
5  Department of Chemical and Petroleum Engineering and Department of Chemistry, University of Kansas, Lawrence, KS, USA; State Key Laboratory of Photocatalysis on Energy and Environment and College of Chemistry, Fuzhou University, Fuzhou, China 
6  Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, NY, USA; Division of Chemistry, Brookhaven National Laboratory, Upton, NY, USA 
Pages
1-11
Publication year
2018
Publication date
Mar 2018
Publisher
Nature Publishing Group
e-ISSN
20411723
Source type
Scholarly Journal
Language of publication
English
DOI
https://doi.org/10.1038/s41467-018-03235-7
ProQuest document ID
2018652278
Copyright
© 2018. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.