Insights into the Mechanism of n-Hexane Reforming over a Single-Site Platinum Catalyst

Zhang, Shuchen; Chen, Luning; Qi, Zhiyuan; Zhuo, Lei; Chen, Jeng-Lung; Pao, Chih-Wen; Su, Ji; Somorjai, Gabor A.

doi:10.1021/jacs.0c07911

Insights into the Mechanism of n-Hexane Reforming over a Single-Site Platinum Catalyst

Journal Article · Mon Sep 14 00:00:00 EDT 2020 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.0c07911· OSTI ID:1779254

^[1]; ^[1]; Qi, Zhiyuan ^[1]; Zhuo, Lei ^[1]; Chen, Jeng-Lung ^[2]; Pao, Chih-Wen ^[2]; Su, Ji ^[1]; ^[3]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
National Synchrotron Radiation Research Center, Hsinchu (Taiwan)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)

We demonstrate that the single-site catalyst Pt₁/CeO₂ greatly enhances the selectivity of cyclization and aromatization in the n-hexane reforming reaction. Specifically, the selectivity of single-site Pt₁/CeO₂ toward both cyclization and aromatization is above 86% at 350 °C. The turnover frequency of Pt₁/CeO₂ is 58.8 h^-1 at 400 °C, which is close to that of Pt cluster/CeO₂ (61.4 h^-1) and much higher than that of Pt nanoparticle/CeO₂ with Pt sizes of 2.5 and 7 nm. On the basis of the catalytic results for methylcyclopentane reforming, the dehydrocyclization and further aromatization of n-hexane are attributed to the prominent adsorption of ring intermediate products on the single-site Pt₁/CeO₂ catalysts. On the other side, with the multiple Pt adjacent active sites, the cluster and nanoparticle Pt/CeO₂ samples favor the C-C bond cracking reaction. Ultimately, this in-depth study unravels the principles of hydrocarbon activation with different Pt sizes and represents a key step toward the rational design of new heterogeneous catalysts.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1779254

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 39 Vol. 142; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Catalysts
Cyclization
Hydrocarbons
Platinum
Selectivity

Insights into the Mechanism of n-Hexane Reforming over a Single-Site Platinum Catalyst

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