During compression, most LHP crystals have their [100] faces oriented normal to, or inclined to, the compression axis, thereby facilitating plastic deformation along the [001] <100> slip system by mechanical twinning. Due to the low attachment energy between them, the [001] planes can also act as cleavage planes. This study demonstrates that knowledge of the crystal structure and slip systems can be used to model the tableting and compaction behavior of molecular crystals, such as LH.

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The objective of the present study was to apply a technique to measure the surface energy of crystalline powders without changing the surface properties by compaction, and to relate such measurements to crystal habit and orientation. The surface free energy of uncompacted L-lysine monohydrochloride dihydrate (LH), determined using a modified sessile-drop method, reflected a combined value for the various faces, and was influenced by the relative size of the faces and the orientation of the crystals. The surface free energy values obtained from contact angle measurements were within the possible range calculated from the crystal structure. Discrepancies between the theoretical estimates of interparticulate cohesive strengths and those measured from the tensile strength of powder compacts were used to estimate the flaw sizes (or gaps between the particles) that act as stress concentrators and reduce the tensile strength of the compacts. The flaw sizes indicate packing and compressibility of the various crystal habits. In the absence of compressive load, compacts made out of the equidimensional crystals have the larger flaw sizes (wider cracks or wider gaps between the particles). At higher compaction pressures, the compacts from long rod-shaped crystals have longer crack lengths. The weakness of the compacts made from the long rods at the higher compaction pressures may be because of the longer crack length along the interparticulate boundary, which may result in a higher stress intensity at the crack tip and increased fracture propensity.

The trend in granule size distribution during the experiment closely followed the predicted model with an initial increase in the weight fraction of the larger granules. This increase was possibly due to extensive breakage of weaker granules and less extensive breakage, as if by attrition, of stronger granules, accompanied by the attachment of dry powder to the cracked surfaces. Eventually, larger granules experience increased impact energy and break. When excess binder is added and, higher volumes of powder reattach to the crack surface, more large granules form leading to granule overgrowth. This model highlights the importance of the probability of impact per unit time interval (ie, the rate of impact), the strength of the granules and the volume of powder that could attach to the cracked surface in high shear granulation processes where significant granule breakage is encountered.