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Insights into the Mechanism of n-Hexane Reforming over a Single Site Platinum Catalyst
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-09-14 , DOI: 10.1021/jacs.0c07911
Shuchen Zhang, Luning Chen, Zhiyuan Qi, Lei Zhuo, Jeng-Lung Chen, Chih-Wen Pao, Ji Su, Gabor A. Somorjai

We demonstrated the single site catalyst Pt1/CeO2 greatly enhanced the selectivity of cyclization and aromatization in the n-hexane reforming reaction. Specifically, the selectivity of single site Pt1/CeO2 towards both cyclization and aromatization is above 86 % at 350 ˚C. The turnover frequency (TOF) of Pt1/CeO2 is 58.8 h-1 at 400 oC, which is close to Pt cluster/CeO2 (61.4 h-1), and much higher than Pt nanoparticle/CeO2 with Pt size of 2.5 nm and 7 nm. Combined with the catalytic results of cyclopentane (MCP) reforming, the dehydrocyclization and further aromatization of n-hexane was attributed to the prominent absorption 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 un-ravels the principles of hydrocarbons activation with differ-ent Pt size and represents a key step towards the rational design of new heterogeneous catalysts.

中文翻译:

单位点铂催化剂上正己烷重整机理的洞察

我们证明了单中心催化剂 Pt1/CeO2 大大提高了正己烷重整反应中环化和芳构化的选择性。具体而言,单中心 Pt1/CeO2 对环化和芳构化的选择性在 350 ˚C 时均高于 86%。Pt1/CeO2 在 400 oC 的转换频率 (TOF) 为 58.8 h-1,接近 Pt 簇/CeO2 (61.4 h-1),远高于 Pt 尺寸为 2.5 nm 和 7纳米。结合环戊烷(MCP)重整的催化结果,正己烷的脱氢环化和进一步芳构化归因于环中间产物在单中心 Pt1/CeO2 催化剂上的显着吸收。另一方面,由于多个 Pt 相邻的活性位点,簇和纳米颗粒 Pt/CeO2 样品有利于 CC 键裂解反应。最终,
更新日期:2020-09-14
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