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

• Published in: Angewandte Chemie (International ed.) 2016-10, Vol.55 (43), p.13441-13445
• Main Authors: Huang, Weixin, Zhang, Shiran, Tang, Yu, Li, Yuting, Nguyen, Luan, Li, Yuanyuan, Shan, Junjun, Xiao, Dequan, Gagne, Raphael, Frenkel, Anatoly I., Tao, Franklin (Feng)
• Format: Article
• Language: English
• Subjects: Catalysts; Chemical industry; Direct conversion; Hydrogen peroxide; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Low temperature; Mathematical analysis; Methane; Methanol; Oxidation; palladium; Phase transitions; Selectivity; single-sites; Temperature effects
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.201604708

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 °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 °C is about 2.78 molecules per Pd1O4 site per second when 2.0 wt % 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. Single site Pd1O4 anchored in microspores of zeolite with 2.0 w % CuO is active for transforming of CH4 to CH3OH in aqueous solution in the temperature range of 50–95 °C. Selectivity for production of CH3OH in this temperature range was found to be 78 %‐86 % at 50–95 °C, offering a clear improvement over harsh alternative conditions.