Low‐Temperature Transformation of Methane to Methanol on Pd1O4 Single Sites Anchored on the Internal Surface of Microporous Silicate. Issue 43 (26th September 2016)

• Record Type: Journal Article
• 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)
• Is Part Of: Angewandte Chemie international edition. Volume 55:Issue 43(2016)
• Page Start: 13441
• Page End: 13445
• Publication Date: 2016-09-26
• Subjects: methane -- methanol -- oxidation -- palladium -- single-sites; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.201604708
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: Direct conversion of methane to chemical feedstocks such as methanol under mild conditions is a challenging but ideal solution for utilization of methane. Pd1 O4 single‐sites anchored on the internal surface of micropores of a microporous silicate exhibit high selectivity and activity in transforming CH4 to CH3 OH at 50–95 °C in aqueous phase through partial oxidation of CH4 with H2 O2 . The selectivity for methanol production remains at 86.4 %, while the activity for methanol production at 95 °C is about 2.78 molecules per Pd1 O4 site per second when 2.0 wt % CuO is used as a co‐catalyst with the Pd1 O4 @ZSM‐5. Thermodynamic calculations suggest that the reaction toward methanol production is highly favorable compared to formation of a byproduct, methyl peroxide. Abstract : Single site Pd1 O4 anchored in microspores of zeolite with 2.0 w % CuO is active for transforming of CH4 to CH3 OH in aqueous solution in the temperature range of 50–95 °C. Selectivity for production of CH3 OH in this temperature range was found to be 78 %‐86 % at 50–95 °C, offering a clear improvement over harsh alternative conditions.