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首页> 外文期刊>ACS catalysis >Synergistic Computational-Experimental Discovery of Highly Selective PtCu Nanocluster Catalysts for Acetylene Semihydrogenation
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Synergistic Computational-Experimental Discovery of Highly Selective PtCu Nanocluster Catalysts for Acetylene Semihydrogenation

机译：乙炔半红细胞催化剂高选择性PTCU纳米光栅催化剂的协同计算实验发现

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摘要

Semihydrogenation of acetylene (SHA) in an ethylene-rich stream is an important process for polymer industries. Presently, Pd-based catalysts have demonstrated good acetylene conversion (X-C2H2), however, at the expense of ethylene selectivity (S-C2H4). In this study, we have employed a systematic approach using density functional theory (DFT) to identify the best catalyst in a Cu-Pt system. The DFT results showed that with a 55 atom system at similar to 1.1 Pt/Cu ratio for Pt28Cu27/Al2O3, the d-band center shifted -2.2 eV relative to the Fermi level leading to electron-saturated Pt, which allows only adsorption of ethylene via a pi-bond, resulting in theoretical 99.7% S-C2H4 at nearly complete X-C2H2. Based on the DFT results, Pt-Cu/Al2O3 (PtCu) and Pt/Al2O3 (Pt) nanocatalysts were synthesized via cluster beam deposition (CBD), and their properties and activities were correlated with the computational predictions. For bimetallic PtCu, the electron microscopy results show the formation of alloys. The bimetallic PtCu catalyst closely mimics the DFT predictions in terms of both electronic structure, as confirmed by X-ray photoelectron spectroscopy, and catalytic activity. The alloying of Pt with Cu was responsible for the high C2H4 specific yield resulting from electron transfer between Cu and Pt, thus making PtCu a promising catalyst for SHA.
机译：富含乙烯流中的乙炔（SHA）的半氢化是聚合物工业的重要方法。目前，Pd基催化剂已经表现出良好的乙炔转化率（X-C2H2），然而，以亚乙基选择性（S-C2H4）为代价。在这项研究中，我们使用了使用密度官能理论（DFT）的系统方法来鉴定Cu-PT系统中的最佳催化剂。 DFT结果表明，对于PT28Cu27 / Al2O3的类似于1.1pt / Cu比的55原子系统，D频带中心相对于导致电子饱和Pt的费米水平偏移-2.2eV，其仅吸附乙烯通过PI-键，在几乎完全X-C2H2处产生理论99.7％S-C2H4。基于DFT结果，通过簇束沉积（CBD）合成PT-Cu / Al 2 O 3（PTCU）和Pt / Al 2 O 3（Pt）纳米催化剂，其性质和活性与计算预测相关。对于双金属PTCU，电子显微镜结果显示了合金的形成。双金属PTCU催化剂在电子结构方面密切地模仿DFT预测，如X射线光电子能谱和催化活性所证实。 Pt与Cu的合金负责Cu和Pt之间的电子转移产生的高C2H4特异性产量，从而使PTCU成为SHA的有望催化剂。

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