CeO2–ZrO2 (CZO) nanoparticles (NPs) have applications in many catalytic reactions, such as methane dry reforming, due to their oxygen cycling ability. Ni doping has been shown to improve the catalytic activity and produces active sites for the decomposition of methane. In this work, Ni:CZO NPs were synthesized via a two-step co-precipitation/molten salt synthesis to compare Ni distribution, oxygen vacancy concentration, and catalytic activity relative to a reference state-of-the-art catalyst prepared by a sol–gel-adsorptive deposition technique. To better understand the dispersion of Ni and oxygen vacancy formation in these materials, the Ni concentration, position, and reaction time were varied in the synthesis. X-ray diffraction (XRD) measurements show a homogeneous, cubic phase with little to no segregation of Ni/NiO. Catalytic activity measurements, performed via a differential scanning calorimetry (DSC)/thermogravimetric analysis (TGA) method, displayed a 5-fold increase in the activity per surface area with an order of magnitude decrease in the coking rate for the particles synthesized by the molten salt method. Additionally, this approach resulted in an order of magnitude increase in oxygen vacancies, which is attributed to the high dispersion of Ni2+ ions in the NP core. This ability of controlling the oxygen vacancies in the lattice is expected to impact other such systems, which utilize the substrate redox cyclability to drive conversion via, e.g., a Mars–van Krevelen mechanism.
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.
We demonstrate that for polyethylene depolymerization with induction heating (IH), using a bifunctional (Pt-or Pt− Sn-containing zeolite) hydrocracking catalyst, we can obtain high hydrocarbon product yields (up to 95 wt % in 2 h) at a relatively low surface temperature (375 °C) and with a tunable product distribution ranging from light gas products to gasoline-to dieselrange hydrocarbons. Four zeolite types [MFI, LTL, CHA(SSZ-13), and TON] were chosen as the supports due to their varying pore sizes and structures. These depolymerization results are obtained at atmospheric pressure and without the use of H 2 and result in an alkane/alkene mixture with virtually no methane, aromatics, or coke formation. We also demonstrate how IH helps overcome diffusional resistances associated with conventional thermal heating and thereby shortens reaction times.
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 Fe 3 O 4 catalysts composed of 28–32 nm diameter nanoparticles. The Fe 3 O 4 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/Fe 3 O 4 , 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/Fe 3 O 4 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.
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