How Thermal Aging Affects Ignition and Combustion Properties of Reactive Al/CuO Nanolaminates: A Joint Theoretical/Experimental Study

The paper reports a joint experimental/theoretical study on the aging of reactive Al/CuO nanolaminates, investigating both structural modifications and combustion properties of aged systems. We first show theoretically that the long-term storage (over several decades) in ambient temperature marginally affects nanolaminates structural properties with an increase in an interfacial layer of only 0.3 nm after 30 years. Then, we observe that the first thermal aging step occurs after 14 days at 200 degrees C, which corresponds to the replacement of the natural Al/CuO interfaces by a proper similar to 11 nm thick amorphous alumina. We show that this aging step does impact the nanolaminates structure, leading, for thin bilayer thicknesses, to a substantial loss of the energetic reservoir: considering a stoichiometric Al/CuO stack, the heat of reaction can be reduced by 6-40% depending on the bilayer thickness ranging from 150 nm (40%) to 1 mu m (6%). The impact of such thermal aging (14 days at 200 degrees C) and interfacial modification on the initiation and combustion properties have been evaluated experimentally and theoretically. Varying Al to CuO ratio of nanolaminates from 1 to 3, we show that ignition time of aged systems does not increase over 10% at initiation power densities superior to 15 W.mm(-2). In contrast, burn rate can be greatly impacted depending on the bilayer thickness: annealing a stoichiometric nanolaminates with a bilayer thickness of 300 nm at 200 degrees C for 14 days lowers its burn rate by similar to 25%, whereas annealing a fuel rich nanolaminates with the same bilayer thickness under the same thermal conditions leads to a burn rate decrease of 20%. When bilayer thickness is greater than 500 nm, the burn rate is not really affected by the thermal aging. Finally, this paper also proposes a time-temperature diagram to perform accelerated thermal aging.