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It was originally called Santa Ana, but on May 10, 1858, was renamed in honor of the French naturalist Aimé Bonpland whose body rests in a mausoleum in the Cemetery of the Holy Cross of Paso de los Libres.
On April 1, 1843, the Madariaga brothers and some more officials crossed the Uruguay River near Uruguaiana, on what would later be known as the 'Paso de los Libres'.