Catalytic dehydrogenation of liquid organic hydrogen carrier dodecahydro-N-ethylcarbazole over palladium catalysts suppo
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RESEARCH ARTICLE
Catalytic dehydrogenation of liquid organic hydrogen carrier dodecahydro-N-ethylcarbazole over palladium catalysts supported on different supports Zhaolu Feng 1 & Xiaomin Chen 2 & Xuefeng Bai 1,3,2 Received: 12 April 2020 / Accepted: 11 June 2020 # Springer-Verlag GmbH Germany, part of Springer Nature 2020
Abstract The system based on liquid organic hydrogen carrier (LOHC) is one of the technologies to solve the problem of hydrogen storage and transportation capacity in large-scale applications. In this paper, the catalytic dehydrogenation of LOHC dodecahydro-Nethylcarbazole (H12-NEC) over supported Pd nanoparticles (NPs) catalyst on four kinds of different supports, such as Pd/C, Pd/ Al2O3, Pd/TiO2, and Pd/SiO2, was studied. It was found from catalyst characterization and dehydrogenation reaction that the volcano-type dependence of the activity on the Pd particle size, catalytic activity improvement with large specific surface area, and high Pd reduction degree indicated that the structure, particle size, and reduction degree of Pd NPs and textural properties of supports had a synergistic effect on the catalytic performance. Among all the catalysts, Pd/C displayed outstanding catalytic performance with the H12-NEC conversion of 99.9% and hydrogen storage capacity of 5.69 wt% at 180 °C after 12 h. The particle size of Pd/C distributes in the range of 1.5–6.0 nm with an average size of 3.0 nm. The results of dehydrogenation reaction kinetics showed that the rate limiting step and rate constant for different catalysts were mainly related to the physicochemical properties and adsorption and activation abilities towards the reactants and intermediates. In terms of the stationarity of dehydrogenation process, Pd/Al2O3 was excellent, indicating that it was best for dehydrogenation of H12-NEC. Keywords Hydrogen storage . Liquid organic hydrogen carrier . Dodecahydro-N-ethylcarbazole . Catalytic dehydrogenation . Pd catalysts . Support
Introduction In recent years, atmospheric pollution has become one of the prominent problems in environmental protection such as acid rain, stratospheric ozone depletion, greenhouse effect, photochemical smog, and haze (Debnath and Mourshed 2018; Dincer 2002; Nicoletti et al. 2015). COx, SOx, NOx, and other harmful substances emitted by the combustion of fossil fuels
Responsible Editor: Santiago V. Luis * Xuefeng Bai [email protected] 1
College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, People’s Republic of China
2
Institute of Petrochemistry, Heilongjiang Academy of Sciences, Harbin 150040, People’s Republic of China
3
School of Chemistry and Material Science, Heilongjiang University, Harbin 150080, People’s Republic of China
are one of the major contributors to atmospheric pollution. In particular, the internal combustion engine has become indispensable machines for production and life of people, but the smoke emitted during their use can cause corresponding air pollution and even bring inflammatory or cancer to pe
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