He founded the University of Buenos Aires, as well as the Theater, Geology, and Medicine Academies and the continent's first museum of natural science.
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On December 14, 1809, he married Juana del Pino y Vera Mujica, daughter of the viceroy of the Río de la Plata, Joaquín del Pino and his second wife, the vicereine Rafaela Francisca de Vera Mujica y López Pintado.
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At that time Prilidiano Pueyrredón was living in Rio with his family, as well as other intellectuals opposed to the regime of Juan Manuel de Rosas including Bernardino Rivadavia, José María Gutiérrez and Juan Bautista Alberdi.
On May 5 he gathered with some of the most influential characters of Buenos Aires —among which were Dalmacio Vélez Sársfield, Valentín Alsina, Tomás Guido and Vicente Fidel López— to propose them to revive the constitutional project of 1826 of Rivadavia in exchange of support for his authority in front of the national government, but the project was rejected.