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

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• 作者：Weixin Huang ; Dr. Shiran Zhang ; Yu Tang ; Yuting Li ; Dr. Luan Nguyen ; Dr. Yuanyuan Li ; Dr. Junjun Shan ; Prof. Dr. Dequan Xiao ; Raphael Gagne ; Prof. Dr. Anatoly I. Frenkel and Prof. Dr. Franklin (Feng) Tao
• 刊名：Angewandte Chemie
• 出版年：2016
• 出版时间：October 17, 2016
• 年：2016
• 卷：128
• 期：43
• 页码：13639-13643
• 全文大小：1187K
• ISSN：1521-3757

文摘

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.