This critical review evaluates the state-of-the-art in propane dehydrogenation catalysis using oxidative and non-oxidative methods, with an emphasis on the sustainability and suitability for process commercialisation.
Pt/KL is the widely accepted catalyst for aromatizing n-hexane by 1,6 ring closure but encounters deactivation issues when aromatizing higher carbon-number feeds; undergoing extensive dealkylation to give unwanted CH4 and unselective products, as well as over-aromatization to form coke. Here, we report the use of a non-acidic MFI zeolite support, containing excess K + beyond ion exchange capacity, well dispersed Pt, and high Pt presence inside the pores, for maximising direct n-alkane aromatization selectivity. TGA, catalyst deactivation studies, and characterizations show that the smaller pore sizes and lack of large cages in the MFI support sterically inhibit coke formation inside the pores (0% compared to 4.9% over Pt/KL for n-octane aromatization), which also reduces dealkylation of ethylbenzene and o-xylene under mild conditions to give a more selective product distribution, 86% selectivity by weight towards C6 ring closure compared to 27% for Pt/KL. Additionally, using NH3-TPD, XPS,CO-DRIFTS, and STEM, we show the contribution of excess K + as an inhibitor of strong acid sites, an indirect Pt electron promoter through improving metal support interaction, and Pt dispersant. This work highlights the alternative use of well-understood zeolitic supports for the highly selective aromatization of n-heptane and n-octane by 1,6 ring closure, increasing the number of potential streams that can undergo direct aromatization, and providing a suitable alternative to Pt/KL.
The production of 2,5‐furandicarboxylic acid (FDCA) from the selective oxidation of 5‐hydroxymethylfurfural (HMF) is a critical step in the production of biopolymers from biomass‐derived materials. In this study, we report the catalytic performance of monometallic Au and Pd, and bimetallic AuPd nanoparticles with different Au : Pd molar ratios synthesised under continuous flow conditions using a millifluidic set‐up and subsequently deposited onto titanium dioxide as the chosen support. This synthetic technique provided a better control over mean particle size and metal alloy composition, that resulted in higher FDCA yield when the catalysts were compared to similar batch‐synthesised materials. A 99% FDCA yield was obtained with the millifluidic‐prepared AuPd/TiO2 catalyst (Au : Pd molar composition of 75 : 25) after being calcined and reduced at 200 °C. The heat treatment caused a partial removal of the protective ligand (polyvinyl alcohol) encapsulating the nanoparticles and so induced stronger metal‐support interactions. The catalyst reusability was also tested, and showed limited particle sintering after five reaction cycles.
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