Continuous Synthesis of Methanol from Methane and Steam over Copper-Mordenite

被引：34

作者：

Jeong, Yu Ri ^{[1
,2
]}

Jung, Hyeonjung ^{[3
]}

Kang, Jongkyu ^{[1
,2
]}

Han, Jeong Woo ^{[3
]}

Park, Eun Duck ^{[1
,2
]}

机构：

[1] Ajou Univ, Dept Chem Engn, Suwon 16499, South Korea

[2] Ajou Univ, Dept Energy Syst Res, Suwon 16499, South Korea

[3] Pohang Univ Sci & Technol POSTECH, Dept Chem Engn, Pohang 37673, South Korea

来源：

ACS CATALYSIS | 2021年 / 11卷 / 03期

基金：

新加坡国家研究基金会;

关键词：

Cu-MOR; methane; methanol; oxidation; zeolite;

D O I：

10.1021/acscatal.0c04592

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：

One-step methane-to-methanol conversion is a "dream reaction" for chemists. In this Letter, continuous direct conversion of methane into methanol with steam under mild conditions using Cu(II)-exchanged mordenite is reported. The methanol production rate depended on the Si/Al ratio, Cu/Al ratio, presence of Bronsted acid sites, and O-2 concentration in the feed. Cu-H-mordenite and Cu-Na-mordenite showed comparable methane conversion rates, but the former provided higher methanol selectivity. At a given Si/Al ratio, the methane conversion rate gave a volcano plot as a function of Cu/Al ratio, and methanol selectivity decreased with increasing Cu/Al ratio. These experimental data and DFT calculation implied that binuclear copper species are more active than mononuclear copper species and that copper oxide clusters are favorable for total oxidation.

引用

页码：1065 / 1070

页数：6

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