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首页> 外文期刊>The journal of physical chemistry, B. Condensed matter, materials, surfaces, interfaces & biophysical >In situ studies of the active sites for the water gas shift reaction over Cu-CeO2 catalysts: Complex interaction between metallic copper and oxygen vacancies of ceria
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In situ studies of the active sites for the water gas shift reaction over Cu-CeO2 catalysts: Complex interaction between metallic copper and oxygen vacancies of ceria

机译：Cu-CeO2催化剂上水煤气变换反应的活性位的原位研究：金属铜与二氧化铈的氧空位之间的复杂相互作用

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摘要

New information about the active sites for the water gas shift (WGS) reaction over Cu-CeO2 systems was obtained using in-situ, time-resolved X-ray diffraction (TR-XRD), X-ray absorption spectroscopy (TR-XAS, Cu K and Cc L-3 edges), and infrared spectroscopy (DRIFTS). Cu-CeO2 nanoparticles prepared by a novel reversed microemulsion method (doped Ce1-xCuxO2 sample) and an impregnation method (impregnated CuOx/ CeO2 sample) were studied. The results from all of the samples indicate that both metallic copper and oxygen vacancies in ceria were involved in the generation of active sites for the WGS reaction. Evidence was found for a synergistic Cu-O-vacancy interaction. This interaction enhances the chemical activity of Cu, and the presence of Cu facilitates the formation of O vacancies in ceria under reaction conditions. Water dissociation occurred on the O-vacancy sites or the CU-O-vacancy interface. No significant amounts of formate were formed on the catalysts during the WGS reaction. The presence of strongly bound carbonates is an important factor for the deactivation of the catalysts at high temperatures. This work identifies for the first time the active sites for the WGS reaction on Cu-CeO2 catalysts and illustrates the importance of in situ structural studies for heterogeneous catalytic reactions.
机译：使用原位，时间分辨X射线衍射（TR-XRD），X射线吸收光谱（TR-XAS）获得了有关Cu-CeO2系统上水煤气变换（WGS）反应活性位点的新信息。 Cu K和Cc L-3边缘）和红外光谱（DRIFTS）。研究了通过新型反向微乳液法（掺杂的Ce1-xCuxO2样品）和浸渍法（浸渍的CuOx / CeO2样品）制备的Cu-CeO2纳米颗粒。来自所有样品的结果表明，二氧化铈中的金属铜和氧空位均参与了WGS反应的活性位点的产生。发现了协同的Cu-O-空位相互作用的证据。这种相互作用增强了Cu的化学活性，并且Cu的存在促进了反应条件下二氧化铈中O空位的形成。水解离发生在O型空位或CU-O型空位界面上。在WGS反应期间，在催化剂上没有形成大量的甲酸。牢固结合的碳酸盐的存在是在高温下催化剂失活的重要因素。这项工作首次确定了Cu-CeO2催化剂上WGS反应的活性位点，并说明了原位结构研究对于非均相催化反应的重要性。

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