Graphite intercalation compounds (GICs) have potential as hydrogen storage materials, from direct physisorption of H2 or as a high surface area nanostructured host for metal hydrides. GICs made from calcium-ammonia solution have demonstrated 3 wt. % H2 uptake but their in-plane structure is elusive due to a lack of long range order. Gravimetry suggests that 2D Ca-NH3 solutions in graphite decompose to form amides, imides and nitrides in sequence; the resultant Ca3N2 is expected to sorb 3.2 wt. % H2. We intend to use MARI as a probe of signature H-N bonds in the amide sequence to determine if and at what temperature these changes occur in the GIC, and compare with the in-situ decomposition of pure Ca-NH3 up to 1200 K to determine its catalytic effect. We will then hydrogenate the resulting samples at room temperature and examine the hydrogen excitations and binding.