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‘Come quickly,” sings Juana Molina with restless energy. These words during the chorus of “Eras” represent the only time that the English language is heard during Molina’s bracing “Wed 21” album. The song’s unconventional beat may keep listeners off balance, but Molina’s hushed delivery will have speakers of any tongue listening closely as if to hear intimate secrets. Delivered in the Argentinean’s native Spanish, the song suggests that her patience may be wearing thin — or that a long wait may be coming to an end.

The latter interpretation best suits Molina’s many fans in Chicago. Although she performed several local dates in the latter half of the 2000’s, Molina has been absent here since previously visiting the Old Town School of Folk Music in 2010. She returns to the school’s Maurer Concert Hall on April 10.

“Wed 21” is Molina’s sixth album, and her first in five years. Songs like “Lo Decido Yo” (“I Decided”) find Molina combining confessional acoustic-based folk and pop with ruthlessly bent synthesizer tones and hypnotic electronic rhythms. The elastic and sinewy “El Oso de la Guarda” (“The Guardian Bear”) eventually disperses into ambient atmospherics. The results are both inviting and disquieting.

The layered harmonies within “Sin Guia No” (“Not Without a Guide”) are deliberately unsettling, painting an atonal picture of uncertainty. Molina sings about being paralyzed by the past and haunted by mistakes. The song represents a struggle that ultimately subsides as the singer finds the strength to move forward without hesitation.

Molina’s captivating performances are typically solo affairs, wherein she defies the singer-with-acoustic guitar stereotype. While twisting the natural sound of her voice and instrument with effects processors, she builds symphonies of electronic and vocal accompaniment by creating and manipulating audio loops.

Molina’s public career began as a comic actress in Argentina, where she remains known for her roles on shows including “La Noticia Rebelde” and “Juana y Sus Hermanas” (“Juana and Her Sisters”). She also gave voice to the Elastigirl character for the Argentine dub of the Disney/Pixar film “The Incredibles.”

Music became the sole focus of Molina’s career in 1996 with the release of her debut album “Rara” (“Weird”). The whisper playing about the edges of Molina’s voice soon garnered comparisons to the singing style of Lisa Germano, and her sense of fearless acoustic experimentation on songs like “Bicho Auto” (“Auto Bug”) traces a thread to Bjork’s category-defying but danceable singles.

♦ Juana Molina, 8 p.m. Apr. 10, Old Town School of Folk Music, 4544 N Lincoln, (773) 728-6000. Tickets $25; SPOTIFY playlist:

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