4.8 Article

Low-Temperature Transformation of Methane to Methanol on Pd1O4 Single Sites Anchored on the Internal Surface of Microporous Silicate

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 55, Issue 43, Pages 13441-13445

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201604708

Keywords

methane; methanol; oxidation; palladium; single-sites

Funding

  1. KU research fund
  2. Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy [DE-SC0014561]
  3. Synchrotron Catalysis Consortium under the U.S. DOE [DE-SC0012335]
  4. [DE-FG02-03ER15476]

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Direct conversion of methane to chemical feedstocks such as methanol under mild conditions is a challenging but ideal solution for utilization of methane. Pd1O4 single-sites anchored on the internal surface of micropores of a microporous silicate exhibit high selectivity and activity in transforming CH4 to CH3OH at 50-95 degrees C in aqueous phase through partial oxidation of CH4 with H2O2. The selectivity for methanol production remains at 86.4%, while the activity for methanol production at 95 degrees C is about 2.78 molecules per Pd1O4 site per second when 2.0wt% CuO is used as a co-catalyst with the Pd1O4@ZSM-5. Thermodynamic calculations suggest that the reaction toward methanol production is highly favorable compared to formation of a byproduct, methyl peroxide.

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