Role of grain boundary structure on diffusion and dissolution during Ni/Al nanolaminate combustion

Abstract

Ni/Al nanolaminates are reactive materials with customizable combustion characteristics. A common approach to synthesize the repeating Ni and Al nanolayers is physical vapor deposition, which often results in columnar grains with ⟨111⟩ texture and grain diameters on the order of a single layer thickness. Changes in grain size have been reported to affect combustion rates, yet the role of individual grain boundaries (GBs) on this process is unclear. Thus, this work investigates the role of the GB structure on atomic diffusion/dissolution and the resulting combustion reaction via molecular dynamics simulations. Nanolaminate combustion is simulated in bicrystal models containing columnar symmetric tilt GBs with ⟨111⟩ misorientation axis perpendicular to the Ni/Al interface. A range of GB misorientation angles is studied, and combustion in a Ni/Al nanolaminate without GBs is simulated for comparison. Combustion in bicrystal models reveals a rise in temperature with an exponential form prior to complete Al melting, while the model without GBs shows a linear temperature increase. Diffusion coefficients are measured for each bicrystal model, and separate Arrhenius fits are used to identify the first three combustion stages. Models containing higher energy GBs generally have higher diffusion coefficients and lower activation energies prior to complete melting of Al, while the GB structure shows little effect on dissolution after the Al layer melts. Thus, the GB structure plays a key role in Ni/Al nanolaminate ignition sensitivity but does not impact runaway combustion.