Carbonized Melamine Cyanurate as a Palladium Catalyst Support for the Dehydrogenation of N-heterocyclic Compounds in LOHC Technology

Autor: Anton P. Koskin, Yurii V. Larichev, Sergey A. Stepanenko, Yury V. Dubinin, Artem B. Ayupov, Andrey A. Saraev, Evgeny A. Suprun, Petr M. Yeletsky
Jazyk: angličtina
Rok vydání: 2023
Předmět:
Zdroj: C, Vol 9, Iss 3, p 83 (2023)
Druh dokumentu: article
ISSN: 2311-5629
DOI: 10.3390/c9030083
Popis: In this work, the use of graphite-like carbon nitride (g-C3N4) with improved texture characteristics for the synthesis of supported palladium catalysts of dehydrogenation of nitrogen-containing heterocycles was studied. This process is key to the creation of liquid organic carrier technology (LOHC) using N-heterocycles as reversibly hydrogenated/dehydrogenated substrates. For the preparation of graphite-like carbon nitride supports with advanced textural characteristics, well-established technology of the melamine cyanurate complex carbonization and standard techniques of adsorption precipitation together with wet impregnation were used for the synthesis of Pd-containing systems. The activity of the synthesized catalysts was studied in decahydroquinoline dehydrogenation. The high weight content of extractable hydrogen (7.2 wt%) and the high extraction rate, respectively, make it possible to consider these substances as the most promising N-heterocyclic compounds for this technology. It was shown that an increase in the specific surface area of g-C3N4 allows for achieving a slightly lower but comparable fineness of palladium particles for the 1 wt% Pd/MCA-500 sample, compared to the standard 1 wt% Pd/C. In this case, the catalytic activity of 1 wt% Pd/MCA-500 in the dehydrogenation of both substrates exceeded the analogous parameter for catalysts supported by nitrogen-free supports. This regularity is presumably associated with the electron-donor effect of surface nitrogen, which favorably affects the dehydrogenation rate as well as the stability of catalytic systems.
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