Spain's Supreme Court said Friday 13 key Catalan separatists would be prosecuted for "rebellion" as Marta Rovira became the latest leading pro-independence figure to flee overseas to escape charges over the region's breakaway bid.
Convictions could result in up to 30 years in prison.
On Friday morning, Judge Pablo Llarena announced that 13 senior Catalan leaders - including Turull and the deposed regional president, Carles Puigdemont - would be charged with rebellion over their roles in last year's unilateral referendum and subsequent declaration of independence.
Also yesterday, the Spanish Supreme Court rejected an appeal to release two other Catalan independence leaders from pre-trial detention while a judge investigates Catalonia's attempt to secede.
He did not set a date for their trial.
Candidate Jordi Turull, a former minister in the previous Catalan government, fell short of the absolute majority needed due to a division within the three parties who seek independence for the northeastern region.
The decision sparked a wave of demonstrations in Barcelona and across Catalonia on Friday.
The deputy leader of the leftwing separatist ERC party, whose chief is now in jail, is now in Switzerland, according to Spanish media.
But the rulings appeared to inflame the protesters and angry crowds confronted lines of riot police protecting Spanish government buildings in Barcelona.
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Four other separatists had already been detained by the Spanish authorities.
Llarena also issued global arrest warrants for former Catalan President Carles Puigdemont, who is in self-imposed exile in Belgium along with four of his former ministers.
It later emerged that she had fled into exile and Spanish media reported that she was in Switzerland.
Turull was one of the five politicians who responded to a court summons, only to find that Judge Llarena had made a decision to send them to jail, denying them bail.
In a broad alliance swinging from centre-right to far left, the separatists failed to elect a new regional president on Thursday after their most radical faction refused to back Turull in a vote of confidence.
The court's decision means the vote on Turull's leadership can not go ahead because his presence is mandatory.
If Turull is not elected in a second vote or that vote does not take place, parties would have to elect another candidate within two months or hold another election, likely in early July.
The ruling also covered Puigdemont's former deputy, Oriol Junqueras; pro-independence civil society campaigners, Jordi Sanchez and Jordi Cuixart and former Catalan interior minister, Joaquim Forn.