Fine-tuning the catalytic activity by applying nitrogen-doped carbon nanotubes as catalyst supports for the hydrogenation of olefins

Milán Szőri,Péter Pekker,Emőke Sikora,Béla Viskolcz,László Vanyorek,Anita Rágyanszki,Béla Fiser,Zsuzsa H. Göndör,Adrienn Kiss,Ferenc Kristály

doi:10.1007/s11144-019-01705-7

Abstract

Nitrogen-free multi-wall carbon nanotubes (MWCNTs) and N-doped bamboo-like carbon nanotubes (BCNTs) were synthesized by using catalytic vapor deposition (CVD) and used as catalyst support materials. Pd, Rh, Ru, and Ir have been deposited onto the nanotubes to achieve metal/nanotube catalysts. The catalytic activity of the samples was fine-tuned by changing the type of support. BCNT supported Pd and Rh (Pd/BCNT, Rh/MWCNT) catalysts were found to be the most active for liquid phase hydrogenation of octadecene amongst these samples. The initial olefin hydrogenation rate of the Pd/BCNT sample was slightly higher than the corresponding MWCNT-supported catalyst. Based on the hydrogenation reaction, the performance of these catalyst had been ranked as follows: Pd/BCNT ≈ Rh/MWCNT > Pd/MWCNT > Rh/BCNT > > Ir/MWCNT > Ru/BCNT > Ir/BCNT > Ru/MWCNT. The structural properties of chemisorbed Pd on MWCNT and N- BCNT were also characterized by means of computational chemical methods in order to shed some light on the nature of metal binding properties of N-doped and undoped surfaces. The calculations shown preference towards the edges of the surfaces which is in good agreement with the experimental findings.

Highlights

The most widely-used industrial catalysts are nowadays activated carbon-based (AC) or zeolite-supported materials, with different noble metals [1,2,3,4,5]
The purity of the multi-wall carbon nanotubes (MWCNTs) and the bamboo-like carbon nanotubes (BCNTs) catalyst supports were evaluated through thermogravimetric analysis (TGA)
The Ir, Rh, Pd, and Rucontaining BCNT- and MWCNT-supported samples were compared through the hydrogenation reaction of 1-octadecene

Summary

Introduction

The most widely-used industrial catalysts are nowadays activated carbon-based (AC) or zeolite-supported materials, with different noble metals [1,2,3,4,5] These catalysts can ensure high product selectivity and efficient conversion, despite the slower reaction rate, which is due to diffusion limitation originated from their microporous structures [6, 7]. MWCNT supported palladium nanoparticles (Pd/MWCNT) is found efficient catalyst for hydrogenation of biomass-derived levulinic acid [13] Due to their extended high-energy edges, bamboo-like carbon nanotubes (BCNTs) are more active CNTs as sorbents than the MWCNTs. There- fore, they are preferred to use in heterogeneous catalysis as a support material [14]

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