The cost of industrial hydrogen production and logistics, and the purity of hydrogen produced from different technologies are two critical aspects for the success of a future hydrogen economy. Here, we present a way to charge the Liquid Organic Hydrogen Carrier (LOHC) dibenzyltoluene (H0-DBT) with industrially relevant, CO2- and CO-containing gas mixtures. As only hydrogen binds to the hydrogen-lean carrier molecule, this process step extracts hydrogen from the gas mixture and binds it selectively to the carrier. Pd on alumina has been identified as the most promising catalyst system for successfully hydrogenating H0-DBT using model gas mixtures resembling the compositions produced in methane reforming and in industrial coke production (up to 50% CO2 and 7% CO). Up to 80% of the hydrogen present in the feedstock mixture could be extracted during the LOHC hydrogenation process. 99.5% of the reacting hydrogen was selectively bound to the H0-DBT LOHC compound. The purity of hydrogen released from the resulting perhydro dibenzyltoluene previously charged with the hydrogen-rich gas mixture proved to be up to 99.99 mol%. (C) 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.