Roles of Solvent in the Catalytic Hydrogen Release from Liquid Organic Hydrogen Carriers: Chemical, Thermodynamical and Technological Aspects

Tran, Ba L.; Bowden, Mark E.; Autrey, Tom; Byun, Mi Yeon; Müller, Karsten

doi:10.1007/s11244-024-01950-8

Title: Roles of Solvent in the Catalytic Hydrogen Release from Liquid Organic Hydrogen Carriers: Chemical, Thermodynamical and Technological Aspects

Journal Article · 20 May 2024 · Topics in Catalysis

DOI: https://doi.org/10.1007/s11244-024-01950-8 · OSTI ID:2447967

^[1];

^[2]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Univ. of Rostock (Germany)

A Liquid Organic Hydrogen Carrier (LOHC) enables the storage and transport of hydrogen at ambient pressures and temperatures in a safe and convenient form using current infrastructure. However, it is challenging to directly compare reactivity and selectivity for hydrogen release, especially when comparing the catalytic efficiencies of neat LOHCs to highly diluted LOHCs in different solvents, reaction conditions, and catalysts. This work evaluates the role of solvents in catalysis and quantifies the energy efficiency of the overall process. The presence of solvent dilutes the volumetric density of available hydrogen, but may be necessary to achieve optimal catalysts stability, reactivity, and product selectivity. With respect to the reaction conditions as determined by thermodynamics, solvents with higher vapor pressures than that of the carrier can cause the erroneous impression of a more favorable reaction equilibrium. Concerning energy efficiency, solvents can result in increased energy demand for hydrogen release as the inert solvent must be heated to reaction temperatures required for release of H₂ from the LOHC. Further, this work recommends that investigations of catalyst reactivity should be carried out at different ratios of solvent to LOHC to understand how the reactivity changes and what the implications are for maximizing energy density and catalyst stability and reactivity. Investigations should also consider how these implications will affect the technical needs of applications intended for the LOHC system. Based on the results of this study, it is advised to focus research activities on LOHC systems with a gravimetric solvent content below about 50% as the thermodynamic disadvantages become very pronounced beyond this threshold.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO)

Grant/Contract Number:: AC05-76RL01830; AC36-08GO28308

OSTI ID:: 2447967

Report Number(s):: PNNL-SA--193431

Journal Information:: Topics in Catalysis, Journal Name: Topics in Catalysis Journal Issue: 13-14 Vol. 67; ISSN 1022-5528

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Roles of Solvent in the Catalytic Hydrogen Release from Liquid Organic Hydrogen Carriers: Chemical, Thermodynamical and Technological Aspects

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