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Cu−Zn Alloy Formation as Unfavored State for Efficient Methanol Catalysts
ChemCatChem ( IF 3.8 ) Pub Date : 2020-05-12 , DOI: 10.1002/cctc.202000777
Elias Frei 1 , Abhijeet Gaur 2 , Henning Lichtenberg 2 , Leon Zwiener 1 , Michael Scherzer 1 , Frank Girgsdies 1 , Thomas Lunkenbein 1 , Robert Schlögl 1, 3
Affiliation  

The active sites of Cu/ZnO‐based catalysts, commercially applied for the hydrogenation of CO2 or CO2‐rich synthesis gas, are still subject of current debates. Generally, the discussion is focused on the nature of the interfacial contact between Cu and ZnO, particularly whether it is rather of oxidic (Cu−ZnO) or alloying (Cu−Zn) character. We report on kinetic investigations on a Cu/ZnO : Al high performance catalyst activated at different temperatures. Incrementally increasing temperature under reductive conditions leads also to increased CuZn‐alloy formation, analyzed by in‐situ X‐ray diffraction, in‐situ X‐ray absorption spectroscopy and high resolution transmission electron microscopy. The combination of the catalytic data and the complementary characterization techniques provide valuable insights on the relevant reaction sites for CH3OH formation. Our results highlight the complexity of the interfacial contact with evidence for Cu−ZnO reaction sites and clarify the negative impact of CuZn alloy formation on the nature of the active site.

中文翻译:

Cu-Zn合金的形成对高效甲醇催化剂的不利影响

商业上用于氢化CO 2或富含CO 2的合成气的基于Cu / ZnO的催化剂的活性位仍然是当前争论的主题。通常,讨论的重点是Cu和ZnO之间的界面接触的性质,特别是它具有氧化性(Cu-ZnO)或合金化(Cu-Zn)特性。我们报告了在不同温度下活化的Cu / ZnO:Al高性能催化剂的动力学研究。在还原条件下温度的逐渐升高也导致CuZn合金形成的增加,通过原位X射线衍射,原位分析X射线吸收光谱法和高分辨率透射电子显微镜。催化数据和互补的表征技术的结合提供了有关CH 3 OH形成相关反应位点的宝贵见解。我们的结果突出了界面接触的复杂性,并提供了有关Cu-ZnO反应位点的证据,并阐明了CuZn合金形成对活性位点性质的负面影响。
更新日期:2020-05-12
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