Novel materials for alkane dehydrogenation: A systematic study on Pt based, subnanometer-sized alloy cluster catalysts

Andreas Hauser, Martin Head-Gordon, Alexis T. Bell

Research output: Contribution to conferenceAbstractResearchpeer-review

Abstract

Variations of the well known Pt/Sn bimetallic nanoparticle theme are analyzed by the application of density functional theory to a series of tetrahedral Pt3X clusters, with element X taken from the P-block, preferably group 14, or from the D-block near group 10. Almost identical cluster geometries allow a systematic investigation of purely electronic effects induced by the replacement of a single Pt atom by element X. Focusing on the propane-to-propene conversion as the desired dehydrogenation reaction we analyze changes in barrier heights for the rate-determining first C-H cleavage step and estimate the product selectivity towards propene by comparing the propene desorption energy to barriers for alternative reaction pathways. We show that two key steps of the reaction mechanism, namely the first C-H cleavage and the propene desorption, vary significantly between different alloys. Promising candidates beside Pt3Sn are Pt3Ir, Pt3Si and Pt3Ge, for which we find higher activity compared to Pt4. Pt3Ir is particularly interesting due to a much weaker adsorption of the product alkene.
Original languageEnglish
Publication statusPublished - 12 Aug 2014
Externally publishedYes
Event248th ACS National Meeting and Exposition - San Francisco, United States
Duration: 10 Apr 201414 Apr 2014
Conference number: 248
http://acselb-529643017.us-west-2.elb.amazonaws.com/chem/248nm/program/divisionindex.php

Conference

Conference248th ACS National Meeting and Exposition
CountryUnited States
CitySan Francisco
Period10/04/1414/04/14
Internet address

Fields of Expertise

  • Advanced Materials Science

Cite this

Hauser, A., Head-Gordon, M., & Bell, A. T. (2014). Novel materials for alkane dehydrogenation: A systematic study on Pt based, subnanometer-sized alloy cluster catalysts. Abstract from 248th ACS National Meeting and Exposition, San Francisco, United States.

Novel materials for alkane dehydrogenation: A systematic study on Pt based, subnanometer-sized alloy cluster catalysts. / Hauser, Andreas; Head-Gordon, Martin; Bell, Alexis T.

2014. Abstract from 248th ACS National Meeting and Exposition, San Francisco, United States.

Research output: Contribution to conferenceAbstractResearchpeer-review

Hauser, A, Head-Gordon, M & Bell, AT 2014, 'Novel materials for alkane dehydrogenation: A systematic study on Pt based, subnanometer-sized alloy cluster catalysts' 248th ACS National Meeting and Exposition, San Francisco, United States, 10/04/14 - 14/04/14, .
Hauser A, Head-Gordon M, Bell AT. Novel materials for alkane dehydrogenation: A systematic study on Pt based, subnanometer-sized alloy cluster catalysts. 2014. Abstract from 248th ACS National Meeting and Exposition, San Francisco, United States.
Hauser, Andreas ; Head-Gordon, Martin ; Bell, Alexis T. / Novel materials for alkane dehydrogenation: A systematic study on Pt based, subnanometer-sized alloy cluster catalysts. Abstract from 248th ACS National Meeting and Exposition, San Francisco, United States.
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N2 - Variations of the well known Pt/Sn bimetallic nanoparticle theme are analyzed by the application of density functional theory to a series of tetrahedral Pt3X clusters, with element X taken from the P-block, preferably group 14, or from the D-block near group 10. Almost identical cluster geometries allow a systematic investigation of purely electronic effects induced by the replacement of a single Pt atom by element X. Focusing on the propane-to-propene conversion as the desired dehydrogenation reaction we analyze changes in barrier heights for the rate-determining first C-H cleavage step and estimate the product selectivity towards propene by comparing the propene desorption energy to barriers for alternative reaction pathways. We show that two key steps of the reaction mechanism, namely the first C-H cleavage and the propene desorption, vary significantly between different alloys. Promising candidates beside Pt3Sn are Pt3Ir, Pt3Si and Pt3Ge, for which we find higher activity compared to Pt4. Pt3Ir is particularly interesting due to a much weaker adsorption of the product alkene.

AB - Variations of the well known Pt/Sn bimetallic nanoparticle theme are analyzed by the application of density functional theory to a series of tetrahedral Pt3X clusters, with element X taken from the P-block, preferably group 14, or from the D-block near group 10. Almost identical cluster geometries allow a systematic investigation of purely electronic effects induced by the replacement of a single Pt atom by element X. Focusing on the propane-to-propene conversion as the desired dehydrogenation reaction we analyze changes in barrier heights for the rate-determining first C-H cleavage step and estimate the product selectivity towards propene by comparing the propene desorption energy to barriers for alternative reaction pathways. We show that two key steps of the reaction mechanism, namely the first C-H cleavage and the propene desorption, vary significantly between different alloys. Promising candidates beside Pt3Sn are Pt3Ir, Pt3Si and Pt3Ge, for which we find higher activity compared to Pt4. Pt3Ir is particularly interesting due to a much weaker adsorption of the product alkene.

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