According to one aspect, a system for midair deployment of an aerostat may include an inflatable structure including a balloon at least partially defining a volume, a reaction vessel defining a chamber in fluid communication with the volume, a fuel package disposed in the chamber, the fuel package including a container and water-reactive aluminum, the container fluidically isolating the water-reactive aluminum from an environment of the chamber, and an actuator actuatable to release the water-reactive aluminum from the container into the environment of the chamber.