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Experimental and Theoretical Understanding of Nitrogen-Doping-Induced Strong Metal-Support Interactions in Pd/TiO2 Catalysts for Nitrobenzene Hydrogenation

机译:氮掺杂诱导的Pd / TiO2催化剂中氮掺杂诱导的强金属支持相互作用的实验与理论认识,用于硝基苯氢化

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摘要

By doping the TiO2 support with nitrogen, strong metal support interactions (SMSI) in Pd/TiO2 catalysts can be tailored to obtain high-performance supported Pd nanoparticles (NPs) in nitrobenzene (NB) hydrogenation catalysis. According to the comparative studies by X-ray diffraction, X-ray photoelectron spectroscopy (XPS), and diffuse reflectance CO FTIR (CO DRIFTS), N-doping induced a structural promoting effect, which is beneficial for the dispersion of Pd species on TiO2. High-angle annular dark-field scanning transmission electron microscopy study of Pd-n on N-doped TiO2 confirmed a predominant presence of sub-2 nm Pd NPs, which are stable under the applied hydrogenation conditions. XPS and CO DRIFTS revealed the formation of strongly coupled Pd N species in Pd/TiO2 with N-doped TiO2 as support. Density functional theory (DFT) calculations over model systems with Pd (n = 1, 5, or 10) clusters deposited on TiO2(101) surface were performed to verify and supplement the experimental observations. In hydrogenation catalysis using NB as a model molecule, Pd NPs on N-doped TiO2 outperformed those on N-free TiO2 in terms of both catalytic activity and stability, which can be attributed to the presence of highly dispersed Pd NPs providing more active sites, and to the formation of Pd N species favoring the dissociative adsorption of the reactant NB and the easier desorption of the product aniline.
机译:通过掺杂用氮气的TiO 2载体,可以根据硝基苯(Nb)氢化催化剂中的高性能支持的Pd纳米颗粒(NPS)在硝基苯(Nb)氢化催化中获得强金属载体相互作用(SMSI)。根据X射线衍射的比较研究,X射线光电子能谱(XPS)和弥漫反射Co FTIR(CO漂移),N-掺杂诱导结构促进效果,这有利于PD种类对TiO2的分散。在N掺杂TiO2上PD-N的高角度环形暗场扫描透射电子显微镜研究证实了亚2 NM PD NP的主要存在,其在施加的氢化条件下稳定。 XPS和CO漂移揭示了在Pd / TiO 2中形成强耦合的PD N物种,用N掺杂TiO2作为载体。进行密度函数理论(DFT)对沉积在TiO 2(101)表面上的Pd(n = 1,5或10)簇的模型系统的计算以验证和补充实验观察。在使用Nb作为模型分子的氢化催化中,在N-掺杂TiO2上的PD NP在催化活性和稳定性方面优于无N-Fiot TiO 2,这可以归因于提供更多活性位点的高度分散的PD NPS,并且形成有利于反应性Nb的解离吸附的PD N物种和产物苯胺的更容易解吸。

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