Origin of the Activity Trend in the Oxidative Dehydrogenation of Ethanol over VOx/CeO2

被引：6

作者：

Zabilska, Anna ^{[1
,2
]}

Zabilskiy, Maxim ^{[1
]}

Nuguid, Rob Jeremiah G. ^{[1
]}

Clark, Adam H. H. ^{[1
]}

Sadykov, Ilia I. I. ^{[1
]}

Nachtegaal, Maarten ^{[1
]}

Kroecher, Oliver ^{[1
,2
]}

Safonova, Olga V. V. ^{[1
]}

机构：

[1] Paul Scherrer Inst, CH-5232 Villigen, Switzerland

[2] Ecole Polytech Fed Lausanne, CH-1015 Lausanne, Switzerland

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2023年 / 62卷 / 18期

基金：

瑞士国家科学基金会;

关键词：

Heterogeneous Catalysis; Oxidative Dehydrogenation; Reaction Mechanisms; Supported Catalysts; X-Ray Absorption Spectroscopy; VANADIUM-OXIDE CATALYSTS; METHANOL OXIDATION; CERIA; REACTIVITY; CLUSTERS;

D O I：

10.1002/anie.202301297

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Supported vanadia (VOx) is a versatile catalyst for various redox processes where ceria-supported VOx have shown to be particularly active in the oxidative dehydrogenation (ODH) of alcohols. In this work, we clarify the origin of the volcano-shaped ethanol ODH activity trend for VOx/CeOx catalysts using operando quick V K- and Ce L-3- edge XAS experiments performed under transient conditions. We quantitatively demonstrate that both vanadium and cerium are synergistically involved in alcohol ODH. The concentration of reversible Ce4+/Ce3+ species was identified as the main descriptor of the alcohol ODH activity. The activity drop in the volcano plot, observed at above ca. 3 V nm(-2) surface loading (ca. 30 % of VOx monolayer coverage), is related to the formation of spectator V4+ and Ce3+ species, which were identified here for the first time. These results might prove to be helpful for the rational optimization of VOx/CeO2 catalysts and the refinement of the theoretical models.

引用

页数：8

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