Enhancing the Activity of Cu-MOR by Water for Oxidation of Methane to Methanol

Author:

Guan Xi’an123ORCID,Wang Yehong1,Liu Xiumei1,Du Hong1ORCID,Guo Xinwen2,Zhang Zongchao1ORCID

Affiliation:

1. Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China

2. State Key Laboratory of Fine Chemicals, The Pennsylvania State University-Dalian University of Technology (PSU-DUT) Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian 116023, China

3. School of chemical engineering, University of Chinese Academy of Sciences, Beijing 100039, China

Abstract

As clean energy, methane has huge reserves and great development potential in the future. Copper zeolites are efficient in the oxidation of methane to methanol. Water has been confirmed as a source of oxygen to regenerate the copper-zeolite active sites to enable selective anaerobic oxidation of methane to methanol. In this work, we report that the methanol yield increased from 36 μmol/g (Cu-MOR1) to 92 μmol/g (Cu-MOR1-water) as a result of water enhancing the activity of copper ion-exchange mordenite catalyst. We show for the first time that water could convert inactive copper species into active copper species during catalyst activation. A combination of the XPS, FTIR, and NMR results indicates that water dissociates and then converts ZCuIIZ into ZCuII(OH) (where Z indicates framework O (Ofw) bonded to one isolated Al in a framework T-site, i.e., 1Al) and simultaneously produces a Brönsted acid site during catalyst activation. This finding can be used to tune the state of copper species and design highly active copper-zeolite catalysts for methane oxidation to methanol.

Funder

National Natural Science Foundation of China

Publisher

MDPI AG

Subject

Physical and Theoretical Chemistry,Catalysis,General Environmental Science

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