Although the scene in "Real Genius" is fictional, there is probably only one pure gas that can be solidified and not cause mass death when it sublimates: nitrogen. Heavier gases would cause asphyxiation. Hydrogen and helium cannot be solidified. Many other gases are poisonous: fluorine, chlorine, carbon monoxide. Oxygen will likely cause the whole building to go up in flames with the smallest spark. Methane, too.
Nitrogen can in principle cause asphyxiation, but there's already so much nitrogen in the atmosphere that you would have to release a whole lot of gas to make an appreciable difference in concentration. Though maybe they had enough; molecules in solids pack well compared to gas.
Perhaps some nitrogen-oxygen alloy, literally frozen air. Can the addition of a small amount of a third substance change the freezing point, like antifreeze (except we want to raise it)?
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