14 October 2021 in Industrial & Engineering Chemistry Research
Low- and high-density polyethylene (LDPE/HDPE) have been selectively depolymerized, without added H2, to C2–C20 + alkanes/alkenes via energy-efficient radio frequency induction heating, coupled with dual-functional heterogeneous Fe3O4 and Ni- or Pt-based catalysts. Fe3O4 was used to locally generate heat when exposed to magnetic fields. Initial results indicate that zeolite-based Ni catalysts are more selective to light olefins, while Ni supported on ceria catalysts are more selective to C7–C14 alkanes/alkenes. LDPE conversions up to 94% were obtained with minimal aromatic, coke, or methane formation which are typically observed with thermal heating. Two depolymerization mechanisms, a reverse Cossee–Arlman mechanism or a random cleavage process, were proposed to account for the different selectivities. The depolymerization process was also tested on commercial LDPE (grocery bags), polystyrene, and virgin HDPE using the Ni on Fe3O4 catalyst, with the LDPE resulting in similar product conversion (∼48%) and selectivity as for virgin LDPE.
1 September 2015 in Journal of Magnetism and Magnetic Materials
17 February 2022 in ACS Applied Nano Materials
Radio frequency (RF) induction heating was compared to conventional thermal heating for the hydrogenation of oleic acid to stearic acid. The RF reaction demonstrated decreased coke accumulation and increased product selectivity at comparable temperatures over mesoporous Fe3O4 catalysts composed of 28–32 nm diameter nanoparticles. The Fe3O4 supports were decorated with Pd and Pt active sites and served as the local heat generators when subjected to an alternating magnetic field. For hydrogenation over Pd/Fe3O4, both heating methods gave similar liquid product selectivities, but thermogravimetric analysis–differential scanning calorimetry measurements showed no coke accumulation for the RF-heated catalyst versus 6.5 wt % for the conventionally heated catalyst. A different trend emerged when hydrogenation over Pt/Fe3O4 was performed. Compared to conventional heating, the RF increased the selectivity to stearic acid by an additional 15%. Based on these results, RF heating acting upon a magnetically susceptible nanoparticle catalyst would also be expected to positively impact systems with high coking rates, for example, nonoxidative dehydrogenations.
14 December 2021 in ACS Applied Nano Materials
18 December 2020 in ChemSusChem
Heat management in catalysis is limited by each material's heat transfer efficiencies, resulting in energy losses despite current thermal engineering strategies. In contrast, induction heating of magnetic nanoparticles (NPs) generates heat at the surface of the catalyst where the reaction occurs, reducing waste heat via dissipation. However, the synthesis of magnetic NPs with optimal heat generation requires interfacial ligands, such as oleic acid, which act as heat sinks. Surface treatments using tetramethylammonium hydroxide (TMAOH) or pyridine are used to remove these ligands before applications in hydrophilic media. In this study, Fe3O4 NPs are surface treated to study the effect of induction heating on the catalytic oxidation of 1‐octanol. Whereas TMAOH was unsuccessful in removing oleic acid, pyridine treatment resulted in a roughly 2.5‐fold increase in heat generation and product yield. Therefore, efficient surfactant removal has profound implications in induction heating catalysis by increasing the heat transfer and available surface sites.
3 May 2019 in The Journal of Physical Chemistry C