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Combined experimental and theoretical study of acetylene semi-hydrogenation over Pd/Al2O3

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Combined experimental and theoretical study of acetylene semi-hydrogenation over Pd/Al2O3. / Gonçalves, Liliana P.L.; Wang, Jianguang; Vinati, Simone; Barborini, Emanuele; Wei, Xian Kui; Heggen, Marc; Franco, Miguel; Sousa, Juliana P.S.; Petrovykh, Dmitri Y.; Soares, Olívia Salomé G.P.; Kovnir, Kirill; Akola, Jaakko; Kolen'ko, Yury V.

In: International Journal of Hydrogen Energy, 2019.

Research output: Contribution to journalArticleScientificpeer-review

Harvard

Gonçalves, LPL, Wang, J, Vinati, S, Barborini, E, Wei, XK, Heggen, M, Franco, M, Sousa, JPS, Petrovykh, DY, Soares, OSGP, Kovnir, K, Akola, J & Kolen'ko, YV 2019, 'Combined experimental and theoretical study of acetylene semi-hydrogenation over Pd/Al2O3', International Journal of Hydrogen Energy. https://doi.org/10.1016/j.ijhydene.2019.04.086

APA

Gonçalves, L. P. L., Wang, J., Vinati, S., Barborini, E., Wei, X. K., Heggen, M., ... Kolen'ko, Y. V. (2019). Combined experimental and theoretical study of acetylene semi-hydrogenation over Pd/Al2O3. International Journal of Hydrogen Energy. https://doi.org/10.1016/j.ijhydene.2019.04.086

Vancouver

Gonçalves LPL, Wang J, Vinati S, Barborini E, Wei XK, Heggen M et al. Combined experimental and theoretical study of acetylene semi-hydrogenation over Pd/Al2O3. International Journal of Hydrogen Energy. 2019. https://doi.org/10.1016/j.ijhydene.2019.04.086

Author

Gonçalves, Liliana P.L. ; Wang, Jianguang ; Vinati, Simone ; Barborini, Emanuele ; Wei, Xian Kui ; Heggen, Marc ; Franco, Miguel ; Sousa, Juliana P.S. ; Petrovykh, Dmitri Y. ; Soares, Olívia Salomé G.P. ; Kovnir, Kirill ; Akola, Jaakko ; Kolen'ko, Yury V. / Combined experimental and theoretical study of acetylene semi-hydrogenation over Pd/Al2O3. In: International Journal of Hydrogen Energy. 2019.

Bibtex - Download

@article{e91fcc494ad3459e92927c708afc150a,
title = "Combined experimental and theoretical study of acetylene semi-hydrogenation over Pd/Al2O3",
abstract = "The semi-hydrogenation of acetylene (C 2 H 2 + H 2 = C 2 H 4 , ΔH = −172 kJ mol −1 )is a well-studied reaction that is important for purification of ethylene, C 2 H 4 , feed used in polyethylene production. Pd-based catalysts are most commonly used to remove acetylene from ethylene feed prior to Ziegler–Natta polymerization because acetylene is a poison for Ziegler–Natta catalysts. New applications of the analogous catalytic processes, with similar requirements for the conversion and selectivity, are considered for the storage of H 2 within the context of the H 2 economy. Here, a combination of experimental and theoretical studies was employed to explore the performance of synthesized Pd nanoparticles and the feasibility of using computational modelling for predicting their catalytic properties. Specifically, a model 5{\%}Pd/Al 2 O 3 nanocatalyst was successfully synthesized using high-throughput flame spray pyrolysis (FSP)method. As a catalyst for acetylene semi-hydrogenation, the material shows high conversion of 97{\%}, a modest selectivity of 62{\%}, and a turnover frequency of ethylene formation of 5 s −1 . The experimental data were further supported by computational modelling of catalytic properties. Results of microkinetic simulations, based on parameters obtained from DFT calculations, over a Pd 30 /Al 2 O 3 (100)model system were correlated with experiments. The insights from this direct comparison of theory and experiments provide indications for future improvements of the theoretical predictions and for novel types of materials with improved catalytic properties.",
keywords = "DFT, Heterogeneous catalysis, Hydrogenation, Kinetics, Modelling, Nanoclusters",
author = "Gon{\cc}alves, {Liliana P.L.} and Jianguang Wang and Simone Vinati and Emanuele Barborini and Wei, {Xian Kui} and Marc Heggen and Miguel Franco and Sousa, {Juliana P.S.} and Petrovykh, {Dmitri Y.} and Soares, {Ol{\'i}via Salom{\'e} G.P.} and Kirill Kovnir and Jaakko Akola and Kolen'ko, {Yury V.}",
year = "2019",
doi = "10.1016/j.ijhydene.2019.04.086",
language = "English",
journal = "International Journal of Hydrogen Energy",
issn = "0360-3199",
publisher = "Elsevier",

}

RIS (suitable for import to EndNote) - Download

TY - JOUR

T1 - Combined experimental and theoretical study of acetylene semi-hydrogenation over Pd/Al2O3

AU - Gonçalves, Liliana P.L.

AU - Wang, Jianguang

AU - Vinati, Simone

AU - Barborini, Emanuele

AU - Wei, Xian Kui

AU - Heggen, Marc

AU - Franco, Miguel

AU - Sousa, Juliana P.S.

AU - Petrovykh, Dmitri Y.

AU - Soares, Olívia Salomé G.P.

AU - Kovnir, Kirill

AU - Akola, Jaakko

AU - Kolen'ko, Yury V.

PY - 2019

Y1 - 2019

N2 - The semi-hydrogenation of acetylene (C 2 H 2 + H 2 = C 2 H 4 , ΔH = −172 kJ mol −1 )is a well-studied reaction that is important for purification of ethylene, C 2 H 4 , feed used in polyethylene production. Pd-based catalysts are most commonly used to remove acetylene from ethylene feed prior to Ziegler–Natta polymerization because acetylene is a poison for Ziegler–Natta catalysts. New applications of the analogous catalytic processes, with similar requirements for the conversion and selectivity, are considered for the storage of H 2 within the context of the H 2 economy. Here, a combination of experimental and theoretical studies was employed to explore the performance of synthesized Pd nanoparticles and the feasibility of using computational modelling for predicting their catalytic properties. Specifically, a model 5%Pd/Al 2 O 3 nanocatalyst was successfully synthesized using high-throughput flame spray pyrolysis (FSP)method. As a catalyst for acetylene semi-hydrogenation, the material shows high conversion of 97%, a modest selectivity of 62%, and a turnover frequency of ethylene formation of 5 s −1 . The experimental data were further supported by computational modelling of catalytic properties. Results of microkinetic simulations, based on parameters obtained from DFT calculations, over a Pd 30 /Al 2 O 3 (100)model system were correlated with experiments. The insights from this direct comparison of theory and experiments provide indications for future improvements of the theoretical predictions and for novel types of materials with improved catalytic properties.

AB - The semi-hydrogenation of acetylene (C 2 H 2 + H 2 = C 2 H 4 , ΔH = −172 kJ mol −1 )is a well-studied reaction that is important for purification of ethylene, C 2 H 4 , feed used in polyethylene production. Pd-based catalysts are most commonly used to remove acetylene from ethylene feed prior to Ziegler–Natta polymerization because acetylene is a poison for Ziegler–Natta catalysts. New applications of the analogous catalytic processes, with similar requirements for the conversion and selectivity, are considered for the storage of H 2 within the context of the H 2 economy. Here, a combination of experimental and theoretical studies was employed to explore the performance of synthesized Pd nanoparticles and the feasibility of using computational modelling for predicting their catalytic properties. Specifically, a model 5%Pd/Al 2 O 3 nanocatalyst was successfully synthesized using high-throughput flame spray pyrolysis (FSP)method. As a catalyst for acetylene semi-hydrogenation, the material shows high conversion of 97%, a modest selectivity of 62%, and a turnover frequency of ethylene formation of 5 s −1 . The experimental data were further supported by computational modelling of catalytic properties. Results of microkinetic simulations, based on parameters obtained from DFT calculations, over a Pd 30 /Al 2 O 3 (100)model system were correlated with experiments. The insights from this direct comparison of theory and experiments provide indications for future improvements of the theoretical predictions and for novel types of materials with improved catalytic properties.

KW - DFT

KW - Heterogeneous catalysis

KW - Hydrogenation

KW - Kinetics

KW - Modelling

KW - Nanoclusters

U2 - 10.1016/j.ijhydene.2019.04.086

DO - 10.1016/j.ijhydene.2019.04.086

M3 - Article

JO - International Journal of Hydrogen Energy

JF - International Journal of Hydrogen Energy

SN - 0360-3199

ER -