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Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions
Open accessAbstract
Catalytic transformation of CH 4 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 CH 4 to acetic acid and methanol through coupling of CH 4, CO and O 2 on single-site Rh 1 O 5 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 Rh 1 O 5 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 CH 4 is activated by Rh 1 O 5 anchored on the wall of micropores of ZSM-5; the formed CH 3 then couples with CO and OH, to produce acetic acid over a low activation barrier.
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Cited by
Cao, L., Luo, Q., Liu, W., Lin, Y., Liu, X., Cao, Y., Zhang, W., Wu, Y., Yang, J., Yao, T., et al. (2018) · Nature Catalysis · doi:10.1038/s41929-018-0203-5 · Cited by 901
Solar-Energy-Mediated Methane Conversion
Song, H., Meng, X., Wang, Z.-J., Liu, H., & Ye, J. (2019) · Joule · doi:10.1016/j.joule.2019.06.023 · Cited by 478
Significant Advances in C1 Catalysis: Highly Efficient Catalysts and Catalytic Reactions
Bao, J., Yang, G., Yoneyama, Y., & Tsubaki, N. (2019) · ACS Catalysis · doi:10.1021/acscatal.8b03924 · Cited by 367
Enabling Specific Photocatalytic Methane Oxidation by Controlling Free Radical Type
Jiang, Y., Li, S., Wang, S., Zhang, Y., Long, C., Xie, J., Fan, X., Zhao, W., Xu, P., Fan, Y., et al. (2023) · Journal of the American Chemical Society · doi:10.1021/jacs.2c13313 · Cited by 341
Metadata
- Authors
- Tang, Y., Li, Y., Fung, V., Jiang, D.-E., Huang, W., Zhang, S., Iwasawa, Y., Sakata, T., Nguyen, L., Zhang, X., Frenkel, A. I., & Tao, F.
- Venue
- Nature Communications
- Published
- 2018-03-26
- Volume
- 9
- Issue
- 1
- Pages
- 1231-1231
- ISSN
- 2041-1723 (ISSN-L)
- OpenAlex
- W2794821307
- Cited by
- 311
- References
- 0
- FWCI
- 7.07
- Type
- journal article
- Language
- en
- Open access
- gold
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- Tang, Y., Li, Y., Fung, V., Jiang, D.-E., Huang, W., Zhang, S., Iwasawa, Y., Sakata, T., Nguyen, L., Zhang, X., Frenkel, A. I., & Tao, F. (2018). Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions. Nature Communications. https://doi.org/10.1038/s41467-018-03235-7
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