Abstract
The catalysts utilized for the dehydrogenation of dibenzyltoluene-based liquid organic hydrogen carriers (LOHCs) remain crucial. The state-of-the-art catalyst for dehydrogenation of dibenzyltoluene-based LOHC still suffers from deactivation and by-product formation. This is crucial in terms of the efficiency of the industrial dehydrogenation plant for hydrogen production, cyclability as well as the cost of replacing the catalyst. The development of catalysts with optimum performance, minimum deactivation and low by-product formation is required to attain the full benefits of the LOHC technology. Therefore, in this study, the effect of Mg and Zn modification on Pt/Al2O3 catalyst is investigated for the catalytic dehydrogenation of perhydro-dibenzyltoluene (H18-DBT). In addition, an assessment of reaction kinetics is also conducted. High dehydrogenation performance was obtained for Mg-doped Pt/Al2O3 using a batch reactor at 300 °C and 6 h reaction time. In this case, the degree of dehydrogenation (dod), productivity and conversion obtained are 100%, 1.84 gH2/gPt/min and 99.9%, respectively. Moreover, the Mg-doped catalyst has resulted in a high turnover frequency (TOF) of 586 min−1 compared to the Zn-doped catalyst (269 min−1) and the undoped catalyst (202 min−1) at the reaction temperature of 300 °C. The amount of by-products increased with an increase in the catalytic activity, with the Pt/Mg-Al2O3 catalyst possessing the highest amount of by-products. The dehydrogenation of H18-DBT followed first-order reaction kinetics. In addition, the activation energy obtained using the Arrhenius model is 102, 130 and 151 kJ/mol for Pt/Al2O3, Pt/Zn-Al2O3 and Pt/Mg-Al2O3, respectively. Although the Mg-doped Pt/Al2O3 shows high activation energy, the higher performance of the catalyst suggests that mass transfer limitations have no major effect on the dehydrogenation reaction under the conditions used.
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