Hi,
The train between Uyuni and Villazon will only cost you time. Stick to busses: it's quickest and easiest to travel from La Paz to Villazon, cross the border on foot, and then go on from La Quiaca to Salta or, if possible, Buenos Aires directly. Service on this route is very frequent: this is one of the major north-south corridors through SA.
Alternatively, the route via Yacuiba is very comfortable, but I think that will take more time.
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