Influence of Nanoscale Intimacy in Bi-Functional Catalysts for CO<sub>2</sub>-Assisted Dehydrogenation of C<sub>5</sub>-Paraffins

oleh: Muhammad Numan, Gayoung Lee, Eunji Eom, Jae Won Shin, Dae-Heung Choi, Changbum Jo

Format: Article
Diterbitkan: MDPI AG 2023-05-01

Deskripsi

In this study, Pt<sub>1</sub>Sn<sub>1</sub> intermetallic nanoparticles (NPs) on SiO<sub>2</sub>/CeO<sub>2</sub>@SiO<sub>2</sub> composites were located either on SiO<sub>2</sub> or on CeO<sub>2</sub>@SiO<sub>2</sub>, thereby varying the average distance (intimacy) between metal sites and CeO<sub>x</sub> sites from “closest” to “nanoscale”. The catalytic performance of these catalysts was compared to dual-bed mixtures of Pt<sub>1</sub>Sn<sub>1</sub>@SiO<sub>2</sub> and CeO<sub>2</sub>@SiO<sub>2</sub> powders, which provided a “milliscale” distance between sites. Several beneficial effects on the catalytic performance of CO<sub>2</sub>-assisted oxidative dehydrogenation of C<sub>5</sub>-paraffins were observed when Pt<sub>1</sub>Sn<sub>1</sub> nanoparticles were located on SiO<sub>2</sub> in nanoscale proximity to the CeO<sub>2</sub> sites, as opposed to Pt and Sn species located on CeO<sub>2</sub>@SiO<sub>2</sub> with the closest proximity and milliscale intimacy between Pt<sub>1</sub>Sn<sub>1</sub> and CeO<sub>2</sub>. The former catalysts exhibited the highest C<sub>5</sub>-paraffin conversion of 32.8%, with a C<sub>5</sub> total olefin selectivity of 68.7%, while the closest-proximity sample had a lower conversion of 17.4%, with a C<sub>5</sub> total olefin selectivity of 20.9%. The FT-IR (Fourier transform infrared spectroscopy) spectroscopic study of the CO adsorption and X-ray photoelectron spectroscopy results revealed that the closest proximity between Pt and Ce inhibited PtSn alloy formation due to their strong interaction. However, for the nanoscale-proximity sample, neighboring CeO<sub>2</sub>@SiO<sub>2</sub> did not disturb Pt<sub>1</sub>Sn<sub>1</sub> intermetallic formation. This strategy can be applied to other CO<sub>2</sub> activation catalysts, instead of CeO<sub>2</sub>@SiO<sub>2</sub>. This paper aims to provide insights into the influence of metal–CeO<sub>x</sub> intimacy in bi-functional catalysts.