The Nuclearity of the Active Site for Methane to Methanol Conversion in Cu-Mordenite: A Quantitative Assessment

被引：185

作者：

Pappas, Dimitrios K. ^{[1
]}

Martini, Andrea ^{[2
,3
,5
]}

Dyballa, Michael ^{[1
,6
,9
]}

Kvande, Karoline ^{[1
]}

Teketel, Shewangizaw ^{[7
]}

Lomachenko, Kirill A. ^{[8
]}

Baran, Rafal ^{[8
]}

Glatzel, Pieter ^{[8
]}

Arstad, Bjornar ^{[6
]}

Berlier, Gloria ^{[2
,3
]}

Lamberti, Carlo ^{[4
,5
]}

Bordiga, Silvia ^{[1
,2
,3
]}

Olsbye, Unni ^{[1
]}

Svelle, Stian ^{[1
]}

Beato, Pablo ^{[7
]}

Borfecchia, Elisa ^{[2
,3
,7
,10
]}

机构：

[1] Univ Oslo, Dept Chem, Ctr Mat Sci & Nanotechnol, 1033 Blindern, N-0315 Oslo, Norway

[2] Univ Turin, Dept Chem, I-10125 Turin, Italy

[3] Univ Turin, INSTM Reference Ctr, I-10125 Turin, Italy

[4] Univ Turin, Dept Phys, I-10125 Turin, Italy

[5] Southern Fed Univ, IRC Smart Mat, Zorge St 5, Rostov Na Donu 344090, Russia

[6] SINTEF Ind, Forskningsveien 1, N-0373 Oslo, Norway

[7] Haldor Topsoe Res Labs, Haldor Topsoes Alle 1, DK-2800 Lyngby, Denmark

[8] European Synchrotron Radiat Facil, 71 Ave Martyrs,CS 40220, F-38043 Grenoble 9, France

[9] Univ Stuttgart, Pfaffenwaldring 55, D-70174 Stuttgart, Germany

[10] Univ Oslo, Dept Chem, Ctr Mat Sci & Nanotechnol SMN, 1033 Blindern, N-0315 Oslo, Norway

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2018年 / 140卷 / 45期

关键词：

MULTIVARIATE CURVE RESOLUTION; H BOND ACTIVATION; COPPER IONS; OXIDATION; ZEOLITES; CU-ZSM-5; CORE; BIS(MU-OXO)DICOPPER; SPECTROSCOPY; REDUCTION;

D O I：

10.1021/jacs.8b08071

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The direct conversion of methane to methanol (MTM) is a reaction that has the potential to disrupt a great part of the synthesis gas-derived chemical industry. However, despite many decades of research, active enough catalysts and suitable processes for industrial application are still not available. Recently, several copper-exchanged zeolites have shown considerable activity and selectivity in the direct MTM reaction. Understanding the nature of the active site in these materials is essential for any further development in the field. Herein, we apply multivariate curve resolution analysis of X-ray absorption spectroscopy data to accurately quantify the fraction of active Cu in Cu-MOR (MOR = mordenite), allowing an unambiguous determination of the active site nuclearity as a dicopper site. By rationalizing the compositional parameters and reaction conditions, we achieve the highest methanol yield per Cu yet reported for MTM over Cu-zeolites, of 0.47 mol/mol.

引用

页码：15270 / 15278

页数：9

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