Continuous partial oxidation of methane to methanol over Cu-SSZ-39 catalysts

被引:14
作者
Pokhrel, Jeewan [1 ]
Shantz, Daniel F. [1 ]
机构
[1] Tulane Univ, Dept Chem & Biomol Engn, 6823 St Charles Ave, New Orleans, LA 70118 USA
关键词
SSZ-39; Copper; Methanol; Methane partial oxidation; SMALL-PORE ZEOLITES; TO-METHANOL; COPPER; CONVERSION; ACTIVATION; CU-ZSM-5; NH3-SCR; OXYGEN; SI/AL; CORE;
D O I
10.1016/j.jcat.2023.03.021
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The direct conversion of methane to methanol using molecular oxygen as the oxidant is a grand challenge in the chemical sciences. Here we describe our efforts in using copper-exchanged SSZ-39 for this chemistry and show it is a promising material for this reaction. Testing in a continuous flow reactor at 225 degrees C, Cu-SSZ-39 showed superior activity for methane partial oxidation compared to Cu-SSZ-13 (site time yields of 26.9 +/- 0.8 mol(CH3OH)center dot mol(Cu)(-1).h(-1) *10(-3) versus 13.2 mol(CH3OH)center dot mol(Cu)(-1).h(-1) *10(-3) respectively). A clear maximum in methanol productivity, both in terms of a mass catalyst basis and copper atom basis is observed for Cu-SSZ-39 at a Cu/Al similar to 0.2. Running this reaction in the absence of oxygen over samples with a Cu/Al > 0.1 the reactivity is markedly lower than that in the presence of oxygen unlike what is observed in SSZ-13. (C) 2023 Elsevier Inc. All rights reserved.
引用
收藏
页码:300 / 308
页数:9
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