Negative Charging of Au Nanoparticles during Methanol Synthesis from CO2/H2 on a Au/ZnO Catalyst: Insights from Operando IR and Near-Ambient-Pressure XPS and XAS Measurements

被引：75

作者：

Abdel-Mageed, Ali M. ^{[1
,5
]}

Klyushin, Alexander ^{[2
,3
,4
]}

Rezvani, Azita ^{[1
]}

Knop-Gericke, Axel ^{[2
,3
]}

Schloegl, Robert ^{[2
,3
]}

Behm, Juergen ^{[1
]}

机构：

[1] Ulm Univ, Inst Surface Chem & Catalysis, D-89069 Ulm, Germany

[2] Fritz Haber Inst, Dept Inorgan Chem, Faradayweg 4, D-14195 Berlin, Germany

[3] Max Planck Inst Chem Energy Convers Heterogeneous, Stiftstr 34-36, D-45470 Mulheim, Germany

[4] Helmholtz Zentrum Berlin Mat & Energie, BESSY 2, Albert Einstein Str 15, D-12489 Berlin, Germany

[5] Cairo Univ, Fac Sci, Dept Chem, Giza 12613, Egypt

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2019年 / 58卷 / 30期

关键词：

Au/ZnO catalyst; homogeneous catalysis; in situ XPS; XANES; methanol synthesis; operando FTIR; CO2; HYDROGENATION; OXIDATION; SUPPORT; SPECTROSCOPY; MECHANISM; CLUSTERS;

D O I：

10.1002/anie.201900150

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The electronic and structural properties of Au/ZnO under industrial and idealized methanol synthesis conditions have been investigated. This was achieved by kinetic measurements in combination with time-resolved operando infrared (DRIFTS) as well as in situ near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) and X-ray absorption near-edge spectroscopy (XANES) measurements at the O K-edge together with high-resolution electron microscopy. The adsorption of CO during the reaction revealed the presence of negatively charged Au nanoparticles/Au sites during the initial phase of the reaction. Near-ambient-pressure XPS and XANES demonstrate the build-up of O vacancies during the reaction, which goes along with a substantial increase in the rate of methanol formation. The results are discussed in comparison with previous findings for Cu/ZnO and Au/ZnO catalysts.

引用

页码：10325 / 10329

页数：5

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