Low-Temperature Methane Combustion over Pd/H-ZSM-5: Active Pd Sites with Specific Electronic Properties Modulated by Acidic Sites of H-ZSM-5

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• 作者：Yang Lou ; Jian Ma ; Wende Hu ; Qiguang Dai ; Li Wang ; Wangcheng Zhan ; Yanglong Guo ; Xiao-Ming Cao ; Yun Guo ; P. Hu ; Guanzhong Lu
• 刊名：ACS Catalysis
• 出版年：2016
• 出版时间：December 2, 2016
• 年：2016
• 卷：6
• 期：12
• 页码：8127-8139
• 全文大小：985K
• ISSN：2155-5435

文摘

Pd/H-ZSM-5 catalysts could completely catalyze CH₄ to CO₂ at as low as 320 °C, while there is no detectable catalytic activity for pure H-ZSM-5 at 320 °C and only a conversion of 40% could be obtained at 500 °C over pure H-ZSM-5. Both the theoretical and experimental results prove that surface acidic sites could facilitate the formation of active metal species as the anchoring sites, which could further modify the electronic and coordination structure of metal species. PdO_x interacting with the surface Brönsted acid sites of H-ZSM-5 could exhibit Lewis acidity and lower oxidation states, as proven by the XPS, XPS valence band, CO-DRIFTS, pyridine FT-IR, and NH₃-TPD data. Density functional theory calculations suggest PdO_x groups to be the active sites for methane combustion, in the form of [AlO₂]Pd(OH)-ZSM-5. The stronger Lewis acidity of coordinatively unsaturated Pd and the stronger basicity of oxygen from anchored PdO_x species are two key characteristics of the active sites ([AlO₂]Pd(OH)-ZSM-5) for methane combustion. As a result, the PdO_x species anchored by Brønsted acid sites of H-ZSM-5 exhibit high performance for catalytic combustion of CH₄ over Pd/H-ZSM-5 catalysts.