Adrian Walkowiak , Lukasz Wolski , Oleg I. Lebedev , Marco Daturi , Maria Ziolek
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引用次数: 0
摘要
近几十年来，人们对了解支撑物成分对氧化过程中金物种反应性的影响产生了浓厚的兴趣。本研究顺应了这一科学趋势，探讨了在混合铁铌氧化物上支撑的金催化剂中加入磷酸盐离子对甲醇氧化的影响。使用 XRD、ICP-OES、DR-UV-Vis、N2 物理吸附、HRTEM、HAADF-STEM、SEM-EDX、XPS、TPD-NH3、TPD-CO2 和原位傅立叶变换红外光谱结合 NO 吸附对所有材料进行了全面表征。使用固定床流动反应器结合气相色谱法和操作傅立叶变换红外-质谱系统对催化剂的活性进行了评估。结果表明，掺磷酸盐的催化剂在铁铌混合氧化物上的活性明显高于不含磷酸盐的样品。这种改善源于电子迁移率的提高、酸性的增强以及金纳米颗粒在前一种催化剂上的优化分布。这一研究成果将有助于开发更高效的金催化剂。
Unraveling the impact of phosphate doping on surface properties and catalytic activity of gold supported on mixed iron-niobium oxide in gas phase methanol oxidation
In recent decades, there has been notable interest in understanding the influence of the support composition on the reactivity of gold species in oxidation processes. This study fits in with this scientific trend and investigates the effects of incorporating phosphate ions into Au catalysts supported on mixed iron-niobium oxides in methanol oxidation. All materials were thoroughly characterized using XRD, ICP-OES, DR-UV-Vis, N2 physisorption, HRTEM, HAADF-STEM, SEM-EDX, XPS, TPD-NH3, TPD-CO2, and in situ FTIR combined with adsorption of NO. Activity of the catalysts was evaluated using a fixed-bed flow reactor combined with gas chromatography and operando FTIR-MS system. It was observed that the phosphate-doped catalyst supported on mixed Fe-Nb oxide exhibited significantly higher activity than phosphate-free sample. This improvement resulted from increased electron mobility, enhanced acidity, and optimized distribution of gold nanoparticles on the former catalyst. Knowledge resulting from this work can lead to the development of more efficient gold catalysts.
期刊介绍：
The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes.
The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods.
The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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