作者
Dimitrios K Pappas, Elisa Borfecchia, Michael Dyballa, Ilia A Pankin, Kirill A Lomachenko, Andrea Martini, Matteo Signorile, Shewangizaw Teketel, Bjørnar Arstad, Gloria Berlier, Carlo Lamberti, Silvia Bordiga, Unni Olsbye, Karl Petter Lillerud, Stian Svelle, Pablo Beato
发表日期
2017/10/25
期刊
Journal of the American Chemical Society
卷号
139
期号
42
页码范围
14961-14975
出版商
American Chemical Society
简介
Cu-exchanged zeolites possess active sites that are able to cleave the C–H bond of methane at temperatures ≤200 °C, enabling its selective partial oxidation to methanol. Herein we explore this process over Cu-SSZ-13 materials. We combine activity tests and X-ray absorption spectroscopy (XAS) to thoroughly investigate the influence of reaction parameters and material elemental composition on the productivity and Cu speciation during the key process steps. We find that the CuII moieties responsible for the conversion are formed in the presence of O2 and that high temperature together with prolonged activation time increases the population of such active sites. We evidence a linear correlation between the reducibility of the materials and their methanol productivity. By optimizing the process conditions and material composition, we are able to reach a methanol productivity as high as 0.2 mol CH3OH/mol Cu …
引用总数
20172018201920202021202220232024235644954485826
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DK Pappas, E Borfecchia, M Dyballa, IA Pankin… - Journal of the American Chemical Society, 2017