The promising midfielder joined the club in 2009 as part of the club's heavy investment in their youth set-up but has opted for first-team football at the Oakwell Stadium
The 18-year-old winger, who can play on either flank, joined the club in 2009 from Benfica as part of the club's strategy to focus on developing foreign talent through their academy, but has left without making a single appearance for the first team.
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"Everyone at LFC would like to wish Toni all the very best for the future."
Silva, who failed to make a single first-team appearance for The Reds, joined League Two side Northampton Town on loan for the latter stage of last season and made 15 appearances.
And it appears that Silva has done enough to convince Barnsley manager Keith Hill that he can make the step up from League Two.
Hill told the Sheffield Star: "He's a very talented player, but he's still raw. We've watched him a few times and we've really been impressed with what we've seen.
"He went on loan to Northampton last season, which was a good experience for him. I spoke to Aidy Boothroyd about him and he agrees that he's an exciting prospect.
The Tykes manager was keen to point out that fans should not expect an immediate impact from their exciting prospect.
He added: "This is a really good signing for the club but there needs to be some patience because he's still a young lad."