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丙烷在 Pt-Cu 双金属催化剂上的脱氢反应:积碳沉积的本质和铜的作用。

Propane dehydrogenation over Pt-Cu bimetallic catalysts: the nature of coke deposition and the role of copper.

机构信息

Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering, Tianjin 300072, China.

出版信息

Nanoscale. 2014 Sep 7;6(17):10000-8. doi: 10.1039/c4nr02143f.

Abstract

This paper describes an investigation of the promotional effect of Cu on the catalytic performance of Pt/Al2O3 catalysts for propane dehydrogenation. We have shown that Pt/Al2O3 catalysts possess higher propylene selectivity and lower deactivation rate as well as enhanced anti-coking ability upon Cu addition. The optimized loading content of Cu is 0.5 wt%, which increases the propylene selectivity to 90.8% with a propylene yield of 36.5%. The origin of the enhanced catalytic performance and anti-coking ability of the Pt-Cu/Al2O3 catalyst is ascribed to the intimate interaction between Pt and Cu, which is confirmed by the change of particle morphology and atomic electronic environment of the catalyst. The Pt-Cu interaction inhibits propylene adsorption and elevates the energy barrier of C-C bond rupture. The inhibited propylene adsorption diminishes the possibility of coke formation and suppresses the cracking reaction towards the formation of lighter hydrocarbons on Pt-Cu/Al2O3, while a higher energy barrier for C-C bond cleavage suppresses the methane formation.

摘要

本文研究了 Cu 对 Pt/Al2O3 催化剂丙烷脱氢催化性能的促进作用。研究表明,添加 Cu 后,Pt/Al2O3 催化剂具有更高的丙烯选择性、更低的失活速率和增强的抗积碳能力。Cu 的最佳负载量为 0.5wt%,可将丙烯选择性提高至 90.8%,丙烯收率达到 36.5%。Pt-Cu/Al2O3 催化剂催化性能和抗积碳能力增强的原因归因于 Pt 和 Cu 之间的紧密相互作用,这可以通过催化剂颗粒形态和原子电子环境的变化得到证实。Pt-Cu 相互作用抑制了丙烯的吸附,并提高了 C-C 键断裂的能垒。抑制丙烯吸附减少了积碳形成的可能性,并抑制了 Pt-Cu/Al2O3 上较轻烃形成的裂解反应,而 C-C 键断裂的更高能垒则抑制了甲烷的形成。

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