Preprint Article Version 1 Preserved in Portico This version is not peer-reviewed

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

Anton P. Koskin
* ORCID logo ,
Yurii V. Larichev
ORCID logo ,
Sergey A. Stepanenko
ORCID logo ,
Yury V. Dubinin
ORCID logo ,
Artem B. Ayupov
,
Evgeny A. Suprun
,
Petr M. Yeletsky
* ORCID logo
Version 1 : Received: 6 July 2023 / Approved: 6 July 2023 / Online: 6 July 2023 (10:22:07 CEST)

A peer-reviewed article of this Preprint also exists.

Koskin, A.P.; Larichev, Y.V.; Stepanenko, S.A.; Dubinin, Y.V.; Ayupov, A.B.; Saraev, A.A.; Suprun, E.A.; Yeletsky, P.M. Carbonized Melamine Cyanurate as a Palladium Catalyst Support for the Dehydrogenation of N-heterocyclic Compounds in LOHC Technology. C 2023, 9, 83. Koskin, A.P.; Larichev, Y.V.; Stepanenko, S.A.; Dubinin, Y.V.; Ayupov, A.B.; Saraev, A.A.; Suprun, E.A.; Yeletsky, P.M. Carbonized Melamine Cyanurate as a Palladium Catalyst Support for the Dehydrogenation of N-heterocyclic Compounds in LOHC Technology. C 2023, 9, 83.

Abstract

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 g-C3N4-mca 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 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.

Keywords

g-C3N4; melamine cyanurate; Pd catalysts; single atom catalysts; hydrogen storage; LOHC; dehydrogenation

Subject

Chemistry and Materials Science, Chemical Engineering

Copyright: This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.

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