The need to drastically reduce CO emissions will lead to the transformation of our current, carbon-based energy system to a more sustainable, renewable-based one. In this process, hydrogen will gain increasing importance as secondary energy vector. Energy storage requirements on the TWh scale (to bridge extended times of low wind and sun harvest) and global logistics of renewable energy equivalents will create additional driving forces toward a future hydrogen economy. However, the nature of hydrogen requires dedicated infrastructures, and this has prevented so far the introduction of elemental hydrogen into the energy sector to a large extent. Recent scientific and technological progress in handling hydrogen in chemically bound form as liquid organic hydrogen carrier (LOHC) supports the technological vision that a future hydrogen economy may work without handling large amounts of elemental hydrogen. LOHC systems are composed of pairs of hydrogen-lean and hydrogen-rich organic compounds that store hydrogen by repeated catalytic hydrogenation and dehydrogenation cycles. While hydrogen handling in the form of LOHCs allows for using the existing infrastructure for fuels, it also builds on the existing public confidence in dealing with liquid energy carriers. In contrast to hydrogen storage by hydrogenation of gases, such as CO or N, hydrogen release from LOHC systems produces pure hydrogen after condensation of the high-boiling carrier compounds. This Account highlights the current state-of-the-art in hydrogen storage using LOHC systems. It first introduces fundamental aspects of a future hydrogen economy and derives therefrom requirements for suitable LOHC compounds. Molecular structures that have been successfully applied in the literature are presented, and their property profiles are discussed. Fundamental and applied aspects of the involved hydrogenation and dehydrogenation catalysis are discussed, characteristic differences for the catalytic conversion of pure hydrocarbon and nitrogen-containing LOHC compounds are derived from the literature, and attractive future research directions are highlighted. Finally, applications of the LOHC technology are presented. This part covers stationary energy storage (on-grid and off-grid), hydrogen logistics, and on-board hydrogen production for mobile applications. Technology readiness of these fields is very different. For stationary energy storage systems, the feasibility of the LOHC technology has been recently proven in commercial demonstrators, and cost aspects will decide on their further commercial success. For other highly attractive options, such as, hydrogen delivery to hydrogen filling stations or direct-LOHC-fuel cell applications, significant efforts in fundamental and applied research are still needed and, hopefully, encouraged by this Account.

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Future energy systems will be determined by the increasing relevance of solar and wind energy. Crude oil and gas prices are expected to increase in the long run, and penalties for CO emissions will become a relevant economic factor. Solar- and wind-powered electricity will become significantly cheaper, such that hydrogen produced from electrolysis will be competitively priced against hydrogen manufactured from natural gas. However, to handle the unsteadiness of system input from fluctuating energy sources, energy storage technologies that cover the full scale of power (in megawatts) and energy storage amounts (in megawatt hours) are required. Hydrogen, in particular, is a promising secondary energy vector for storing, transporting, and distributing large and very large amounts of energy at the gigawatt-hour and terawatt-hour scales. However, we also discuss energy storage at the 120-200-kWh scale, for example, for onboard hydrogen storage in fuel cell vehicles using compressed hydrogen storage. This article focuses on the characteristics and development potential of hydrogen storage technologies in light of such a changing energy system and its related challenges. Technological factors that influence the dynamics, flexibility, and operating costs of unsteady operation are therefore highlighted in particular. Moreover, the potential for using renewable hydrogen in the mobility sector, industrial production, and the heat market is discussed, as this potential may determine to a significant extent the future economic value of hydrogen storage technology as it applies to other industries. This evaluation elucidates known and well-established options for hydrogen storage and may guide the development and direction of newer, less developed technologies.

Our contribution demonstrates that hydrogen storage in stationary Liquid Organic Hydrogen Carrier (LOHC) systems becomes much simpler and significantly more efficient if both, the LOHC hydrogenation and the LOHC dehydrogenation reaction are carried out in the same reactor using the same catalyst.

The catalytic hydrogenation of the LOHC compound dibenzyltoluene (H0-DBT) was investigated by 1 H NMR spectroscopy in order to elucidate the reaction pathway of its charging process with hydrogen in the