4.7 Article

Structure sensitivity reaction of chloroform hydrodechlorination to light olefins using Pd catalysts supported on carbon nanotubes and carbon nanofibers

期刊

JOURNAL OF COLLOID AND INTERFACE SCIENCE
卷 648, 期 -, 页码 427-439

出版社

ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcis.2023.05.169

关键词

Hydrodechlorination; Chloroform; Olefins; CNT/CNF; Palladium; Electron density

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This study investigates the upgrading of wasted chloroform for the production of olefins using different catalysts prepared with different precursors. The results show that PdCl-based catalysts demonstrate electron transfer from the support to Pd nanoparticles, which is not observed in PdN-based catalysts. The catalyst with the smallest and well-dispersed Pd nanoparticles on CNT exhibits the highest activity and selectivity to olefins, while the other catalysts suffer from lower selectivity and activity due to the formation of Pd carbides on larger Pd nanoparticles.
The upgrading of wasted chloroform in hydrodechlorination for the production of olefins such as ethylene and propylene is studied by employing four catalysts (PdCl/CNT, PdCl/CNF, PdN/CNT, and PdN/CNF) prepared by different precursors (PdCl2 and Pd(NO3)2) supported on carbon nanotubes (CNT) or carbon nanofibers (CNF). TEM and EXAFS-XANES results confirm that Pd nanoparticle size increases in the order: PdCl/CNT < PdCl/CNF similar to PdN/CNT < PdN/CNF, descending the electron density of Pd nanoparticles in the same order. It illustrates that PdCl-based catalysts show donation of electrons from support to Pd nanoparticles, which is not observed in PdN-based catalysts. Moreover, this effect is more evident in CNT. The smallest and well-dispersed Pd nanoparticles (NPs) on PdCl/CNT with high electron density favor an excellent and stable activity and a remarkable selectivity to olefins. In contrast, the other three catalysts show lower selectivity to olefins and lower activities which suffer strong deactivation due to the formation of Pd carbides on their larger Pd nanoparticles with lower electron density, compared to PdCl/CNT.

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