Anchoring of palladium nanoparticles on N-doped mesoporous carbon.
Anchoring of palladium nanoparticles on N-doped mesoporous carbon.
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DOI：
10.1039/d0cp03234d
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发表时间：
2020-09
期刊：
影响因子：
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通讯作者：
Lisa Warczinski;Bin Hu;Till Eckhard;B. Peng;M. Muhler;C. Hättig
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作者：
Lisa Warczinski;Bin Hu;Till Eckhard;B. Peng;M. Muhler;C. Hättig
在含氮介孔碳上沉积的钯纳米粒子是一种具有高选择性和高效率催化加氢反应的新型催化剂。为了设计和利用这些新型催化剂，了解N掺杂对金属-载体相互作用的影响是至关重要的。用实验(X射线光电子能谱)和计算(密度泛函理论)相结合的方法确定了优先吸附位置，并对相应的金属-载体相互作用给出了详细的解释。结果表明，吡啶N原子是Pd纳米粒子在含氮介孔碳上的优先吸附中心，通过N-Lp-Pd dσ和N-Lp-Pd S以及Pd dπ-π*电荷转移通过孤对与Pd原子相互作用，从而改变了Pd的氧化态。我们的结果证明了含有Pd0和Pd2+中心的双功能钯纳米粒子的存在。
Pd nanoparticles deposited on nitrogen-doped mesoporous carbon are promising catalysts for highly selective and effective catalytic hydrogenation reactions. To design and utilize these novel catalysts, it is essential to understand the effect of N doping on the metal-support interactions. A combined experimental (X-ray photoelectron spectroscopy) and computational (density functional theory) approach is used to identify preferential adsorption sites and to give detailed explanations of the corresponding metal-support interactions. Pyridinic N atoms turned out to be the preferential adsorption sites for Pd nanoparticles on nitrogen-doped mesoporous carbon, interacting through their lone pairs (LPs) with the Pd atoms via N-LP - Pd dσ and N-LP - Pd s and Pd dπ - π* charge transfer, which leads to a change in the Pd oxidation state. Our results evidence the existence of bifunctional palladium nanoparticles containing Pd0 and Pd2+ centers.