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Importance of Metal–Support Interactions for CO2 Hydrogenation: An Operando Near-Ambient Pressure X-ray Photoelectron Spectroscopy Study on Gold-Loaded In2O3 and CeO2 Catalysts
The Journal of Physical Chemistry Letters ( IF 5.7 ) Pub Date : 2024-04-30 , DOI: 10.1021/acs.jpclett.4c00653
Marc Ziemba 1 , Jakob Weyel 1 , Patrick Zeller 2, 3 , Jan Welzenbach 1 , Anna Efimenko 4, 5 , Michael Hävecker 3, 6 , Christian Hess 1
Affiliation  

Metal–support interactions, which are essential for the design of supported metal catalysts, used, e.g., for CO2 activation, are still only partially understood. In this study of gold-loaded In2O3 and CeO2 catalysts during CO2 hydrogenation using near-ambient pressure X-ray photoelectron spectroscopy, supported by near edge X-ray absorption fine structure, we demonstrate that the role of the noble metal strongly depends upon the choice of the support material. Temperature-dependent analyses of X-ray photoelectron spectra under reaction conditions reveal that gold is reduced on CeO2, enabling direct H2 activation, but oxidized on In2O3, leading to decreased activity of Au/In2O3 compared to bare In2O3. At elevated temperatures, the catalytic activity of the In2O3 catalysts strongly increases as a result of facilitated CO2 and (In2O3-based) H2 activation, while the catalytic activity of Au/CeO2 is limited by reoxidation by CO2. Our results underline the importance of operando studies for understanding metal–support interactions to enable a rational support selection in the future.

中文翻译:

金属-载体相互作用对于 CO2 加氢的重要性:载金 In2O3 和 CeO2 催化剂的近常压 X 射线光电子能谱研究

金属-载体相互作用对于设计用于例如CO 2活化的负载型金属催化剂至关重要,但人们对金属-载体相互作用的了解仍然只有部分。在这项对 CO 2加氢过程中负载金的 In 2 O 3和 CeO 2催化剂的研究中,我们使用近环境压力 X 射线光电子能谱,在近边缘 X 射线吸收精细结构的支持下,证明了贵金属的作用很大程度上取决于支撑材料的选择。反应条件下 X 射线光电子能谱的温度依赖性分析表明,金在 CeO 2上被还原,从而能够直接激活 H 2,但在 In 2 O 3上被氧化,导致 Au/In 2 O 3的活性与裸露相比降低在2 O 3。在升高的温度下,由于促进了CO 2和(In 2 O 3基)H 2活化,In 2 O 3催化剂的催化活性强烈增加,而Au/CeO 2的催化活性受到再氧化的限制二氧化碳2。我们的结果强调了操作研究对于理解金属-支撑相互作用的重要性,以实现未来合理的支撑选择。
更新日期:2024-04-30
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