Hydrogen has the highest gravimetric energy density of any energy carrier and produces water as the only oxidation product, making it extremely attractive for both transportation and stationary power applications. However, its low volumetric energy density causes considerable difficulties, inspiring intense efforts to develop chemical-based storage using metal hydrides, liquid organic hydrogen carriers and sorbents. The controlled uptake and release of hydrogen by these materials can be described as a series of challenges: optimal properties fall within a narrow range, can only be found in few materials and often involve important trade-offs. In addition, a greater understanding of the complex kinetics, mass transport and microstructural phenomena associated with hydrogen uptake and release is needed. The goal of this Perspective is to delineate potential use cases, define key challenges and show that solutions will involve a nexus of several subdisciplines of chemistry, including catalysis, data science, nanoscience, interfacial phenomena and dynamic or phase-change materials.
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We gratefully acknowledge research support from the Hydrogen Materials Advanced Research Consortium (HyMARC), which was established as part of the Energy Materials Network under the US DOE Office of Energy Efficiency and Renewable Energy’s Hydrogen and Fuel Cell Technologies Office, under contract numbers DE-AC04-94AL85000 and DE-AC52-07NA27344. Sandia National Laboratories is a multi-mission laboratory managed and operated by National Technology and Engineering Solutions of Sandia—a wholly owned subsidiary of Honeywell International—for the US DOE’s National Nuclear Security Administration under contract DE-NA-0003525. The Pacific Northwest National Laboratory is operated by Battelle for the US DOE under contract DE-AC05-76RL01830.
The authors declare no competing interests.
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Extended Data Fig. 1 Linear regression of entropy and enthalpy of dehydrogenation for bulk and nanoscale hydrides.
Figure 1 shows linear least-squares fits to the thermodynamic data for (a) bulk and (b) nanoscale hydrides. The bulk data, which are a subset of the full HydPARK database10, at best show a weak correlation between the entropy ΔS° and enthalpy ΔH° of H2 dehydrogenation, as indicated by the low values of R2 and the Spearman Rank Correlation Coefficient R. Excluding outlier compositions, as detailed in Ref. 10, improves the fit somewhat, yielding R2 = 0.42 and R=0.68 across the entire ML-ready HydPARK dataset, suggesting a moderate correlation. In contrast, the data for nanoscale hydrides, although admittedly limited, exhibit a fairly strong correlation, with R2 = 0.738 and R = 0.891. Within specific hydride classes, stronger ΔH° and ΔS° correlations can be found. For example, for nano-PdH R2 = 0.954 and R = 0.939 and for bulk AB materials R2 = 0.924 and R = 0.964.
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Allendorf, M.D., Stavila, V., Snider, J.L. et al. Challenges to developing materials for the transport and storage of hydrogen. Nat. Chem. 14, 1214–1223 (2022). https://doi.org/10.1038/s41557-022-01056-2