Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions
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.
- Authors:
-
- Univ. of Kansas, Lawrence, KS (United States). Dept. of Chemical and Petroleum Engineering. Dept. of Chemistry
- Univ. of California, Riverside, CA (United States). Dept. of Chemistry
- Univ. of Kansas, Lawrence, KS (United States). Dept. of Chemical and Petroleum Engineering. Dept. of Chemistry; Univ. of Notre Dame, IN (United States). Dept. of Chemistry and Biochemistry
- Univ. of Electro-Communications, Chofu (Japan). Innovation Research Center for Fuel Cells. Graduate School of Informatics and Engineering
- Univ. of Kansas, Lawrence, KS (United States). Dept. of Chemical and Petroleum Engineering. Dept. of Chemistry; Fuzhou Univ. (China). State Key Lab. of Photocatalysis on Energy and Environment. College of Chemistry
- Stony Brook Univ., NY (United States). Dept. of Materials Science and Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Division of Chemistry
- Publication Date:
- Research Org.:
- Univ. of Kansas, Lawrence, KS (United States); Stony Brook Univ., NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1499949
- Grant/Contract Number:
- FG02-03ER15476; SC0014561
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 9; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; carbon capture and storage; catalytic mechanisms; heterogeneous catalysis
Citation Formats
Tang, Yu, Li, Yuting, Fung, Victor, Jiang, De-en, Huang, Weixin, Zhang, Shiran, Iwasawa, Yasuhiro, Sakata, Tomohiro, Nguyen, Luan, Zhang, Xiaoyan, Frenkel, Anatoly I., and Tao, Franklin. Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions. United States: N. p., 2018.
Web. doi:10.1038/s41467-018-03235-7.
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. Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions. United States. https://doi.org/10.1038/s41467-018-03235-7
Tang, Yu, Li, Yuting, Fung, Victor, Jiang, De-en, Huang, Weixin, Zhang, Shiran, Iwasawa, Yasuhiro, Sakata, Tomohiro, Nguyen, Luan, Zhang, Xiaoyan, Frenkel, Anatoly I., and Tao, Franklin. Mon .
"Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions". United States. https://doi.org/10.1038/s41467-018-03235-7. https://www.osti.gov/servlets/purl/1499949.
@article{osti_1499949,
title = {Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions},
author = {Tang, Yu and Li, Yuting and Fung, Victor and Jiang, De-en and Huang, Weixin and Zhang, Shiran and Iwasawa, Yasuhiro and Sakata, Tomohiro and Nguyen, Luan and Zhang, Xiaoyan and Frenkel, Anatoly I. and Tao, Franklin},
abstractNote = {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.},
doi = {10.1038/s41467-018-03235-7},
journal = {Nature Communications},
number = ,
volume = 9,
place = {United States},
year = {Mon Mar 26 00:00:00 EDT 2018},
month = {Mon Mar 26 00:00:00 EDT 2018}
}
Web of Science
Figures / Tables:
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