In operando visualization of hydride-graphite composites during cyclic hydrogenation by high-resolution neutron imaging

• Hydrogenation of hydride-graphite composites (HGC) is visualized in operando by neutron imaging.
• Unexpected activation of HGCs through formation of active regions is examined.
• Reaction fronts inside HGCs are visualized for the first time.
• Fast loading and unloading of HGC with hydrogen is realized (<1 min).

Hydrogen solid-state storage in metal hydrides has attracted remarkable attention within the past decades due to their high volumetric storage densities at low operating pressures. In particular, recently emerged hydride-graphite composites (HGC) can enable a safe, reliable and very compact hydrogen storage solution for various applications. In this regard, only little is known about the activation behavior of such HGC, their cycle stability and degradation effects. Because of the high sensitivity to hydrogen, neutron imaging offers a distinctive approach to examine in operando reaction fronts, swelling effects and microstructural changes of hydrogen absorbing materials with high spatial and temporal resolution. In this contribution, a comprehensive analysis of various phenomena during activation and cycling of HGC based on a Ti–Mn hydrogen absorbing alloy and expanded natural graphite is reported for the first time. A neutron radiography and tomography set-up with a spatial resolution down to 7 μm was utilized allowing highest detection precision. During initial hydrogenation, regions with enhanced reactivity are observed which contradicts a theoretically expected homogeneous reactivity inside the HGC. These active regions grow with the number of hydrogenation-dehydrogenation cycles until the whole HGC volume uniformly participates in the hydrogen sorption reaction. With regard to long-term hydrogenation-dehydrogenation cycling, inhomogeneous swelling effects were observed from which essential conclusions for technical HGC-based tank systems can be derived.

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