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Methylcyclohexane (MCH) serves as an ideal hydrogen carrier in hydrogen storage and transportation process. In the continuous production of hydrogen from MCH dehydrogenation, the rational design of energy-efficient catalytic way with good performance remains an enormous challenge. Herein, an internal electric heating (IEH) assisted mode was designed and proposed by the directly electrical-driven catalyst using the resistive heating effect. The Pt/Al2O3 on Fe foam (Pt/Al2O3/FF) with unique three-dimensional network structure was constructed. The catalysts were studied in a comprehensive way including X-ray diffraction (XRD), scanning electron microscopy (SEM)-mapping, in situ extended X-ray absorption fine structure (EXAFS), and in situ CO-Fourier transform infrared (FTIR) measurements. It was found that the hydrogen evolution rate in IEH mode can reach up to above 2060 mmol·gPt−1·min−1, which is 2–5 times higher than that of reported Pt based catalysts under similar reaction conditions in conventional heating (CH) mode. In combination with measurements from high-resolution infrared thermometer, the equations of heat transfer rate, and reaction heat analysis results, the Pt/Al2O3/FF not only has high mass and heat transfer ability to promote catalytic performance, but also behaves as the heating component with a low thermal resistance and heat capacity offering a fast temperature response in IEH mode. In addition, the chemical adsorption and activation of MCH molecules can be efficiently facilitated by IEH mode, proved by the operando MCH-FTIR results. Therefore, the as-developed IEH mode can efficiently reduce the heat and mass transfer limitations and prominently boost the dehydrogenation performance, which has a broad application potential in hydrogen storage and other catalytic reaction processes.
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