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

Tutkimustuotosvertaisarvioitu

Standard

Synergistic Computational-Experimental Discovery of Highly Selective PtCu Nanocluster Catalysts for Acetylene Semihydrogenation. / Ayodele, Olumide Bolarinwa; Cai, Rongsheng; Wang, Jianguang; Ziouani, Yasmine; Liang, Zhifu; Spadaro, Maria Chiara; Kovnir, Kirill; Arbiol, Jordi; Akola, Jaakko; Palmer, Richard E.; Kolen'Ko, Yury V.

julkaisussa: ACS CATALYSIS, 2019, s. 451-457.

Tutkimustuotosvertaisarvioitu

Harvard

Ayodele, OB, Cai, R, Wang, J, Ziouani, Y, Liang, Z, Spadaro, MC, Kovnir, K, Arbiol, J, Akola, J, Palmer, RE & Kolen'Ko, YV 2019, 'Synergistic Computational-Experimental Discovery of Highly Selective PtCu Nanocluster Catalysts for Acetylene Semihydrogenation', ACS CATALYSIS, Sivut 451-457. https://doi.org/10.1021/acscatal.9b03539

APA

Ayodele, O. B., Cai, R., Wang, J., Ziouani, Y., Liang, Z., Spadaro, M. C., ... Kolen'Ko, Y. V. (2019). Synergistic Computational-Experimental Discovery of Highly Selective PtCu Nanocluster Catalysts for Acetylene Semihydrogenation. ACS CATALYSIS, 451-457. https://doi.org/10.1021/acscatal.9b03539

Vancouver

Author

Ayodele, Olumide Bolarinwa ; Cai, Rongsheng ; Wang, Jianguang ; Ziouani, Yasmine ; Liang, Zhifu ; Spadaro, Maria Chiara ; Kovnir, Kirill ; Arbiol, Jordi ; Akola, Jaakko ; Palmer, Richard E. ; Kolen'Ko, Yury V. / Synergistic Computational-Experimental Discovery of Highly Selective PtCu Nanocluster Catalysts for Acetylene Semihydrogenation. Julkaisussa: ACS CATALYSIS. 2019 ; Sivut 451-457.

Bibtex - Lataa

@article{5a486705206e45969da2e37497319220,
title = "Synergistic Computational-Experimental Discovery of Highly Selective PtCu Nanocluster Catalysts for Acetylene Semihydrogenation",
abstract = "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 (XC2H2), however, at the expense of ethylene selectivity (SC2H4). 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 ∼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 π-bond, resulting in theoretical 99.7{\%} SC2H4 at nearly complete XC2H2. 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.",
keywords = "alloys, cluster beam deposition, hydrogenation, microkinetic model, nanoclusters",
author = "Ayodele, {Olumide Bolarinwa} and Rongsheng Cai and Jianguang Wang and Yasmine Ziouani and Zhifu Liang and Spadaro, {Maria Chiara} and Kirill Kovnir and Jordi Arbiol and Jaakko Akola and Palmer, {Richard E.} and Kolen'Ko, {Yury V.}",
year = "2019",
doi = "10.1021/acscatal.9b03539",
language = "English",
pages = "451--457",
journal = "ACS CATALYSIS",
issn = "2155-5435",

}

RIS (suitable for import to EndNote) - Lataa

TY - JOUR

T1 - Synergistic Computational-Experimental Discovery of Highly Selective PtCu Nanocluster Catalysts for Acetylene Semihydrogenation

AU - Ayodele, Olumide Bolarinwa

AU - Cai, Rongsheng

AU - Wang, Jianguang

AU - Ziouani, Yasmine

AU - Liang, Zhifu

AU - Spadaro, Maria Chiara

AU - Kovnir, Kirill

AU - Arbiol, Jordi

AU - Akola, Jaakko

AU - Palmer, Richard E.

AU - Kolen'Ko, Yury V.

PY - 2019

Y1 - 2019

N2 - 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 (XC2H2), however, at the expense of ethylene selectivity (SC2H4). 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 ∼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 π-bond, resulting in theoretical 99.7% SC2H4 at nearly complete XC2H2. 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.

AB - 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 (XC2H2), however, at the expense of ethylene selectivity (SC2H4). 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 ∼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 π-bond, resulting in theoretical 99.7% SC2H4 at nearly complete XC2H2. 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.

KW - alloys

KW - cluster beam deposition

KW - hydrogenation

KW - microkinetic model

KW - nanoclusters

U2 - 10.1021/acscatal.9b03539

DO - 10.1021/acscatal.9b03539

M3 - Article

SP - 451

EP - 457

JO - ACS CATALYSIS

JF - ACS CATALYSIS

SN - 2155-5435

ER -