4.8 Article

Synergistic Computational-Experimental Discovery of Highly Selective PtCu Nanocluster Catalysts for Acetylene Semihydrogenation

期刊

ACS CATALYSIS
卷 10, 期 1, 页码 451-457

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b03539

关键词

microkinetic model; hydrogenation; nanoclusters; alloys; cluster beam deposition

资金

  1. European Union's Horizon 2020 research and innovation program through the CritCat Project [686053]
  2. Generalitat de Catalunya [2017 SGR 327]
  3. Spanish MINECO project [ENE2017-85087-C3]
  4. Severo Ochoa program from Spanish MINECO [SEV-2017-0706]
  5. CERCA Programme/Generalitat de Catalunya
  6. MINECO SO FPI Ph.D. grant [SEV-2013-0295-17-1]
  7. European Union's Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant [754510]
  8. EPSRC [EP/K006061/2, EP/E005918/1, EP/D049245/1, EP/K006061/1, EP/E004563/1, EP/D037794/1] Funding Source: UKRI

向作者/读者索取更多资源

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.

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