Catalonian officials said Spain's Guardia Civil, or paramilitary national police, searched several government departments, including the offices of the presidency, economic affairs, and foreign relations on Wednesday morning.
Catalonia's pro-separatist president Carles Puigdemont accused the Spanish government of imposing a "de facto state of emergency" in the region, with a series of measures to prevent what Madrid sees as an illegal independence referendum taking place.
Spain's Constitutional Court says it will fine 22 members of an electoral board overseeing Catalonia's planned independence referendum between 6,000 ($7,200) and 12,000 euros a day as long as they continue disobeying court rulings suspending the October 1 vote.
Spain has discreetly hired ferries to be moored in the Port of Barcelona as temporary housing for possibly thousands of police specially deployed to keep order in rebel Catalonia and help suppress an illegal independence referendum.
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It was the first time the promoters of the referendum had acknowledged their plans were in doubt, although Junqueras said he was convinced voters would still turn out in numbers.
He also stressed that the referendum would go ahead despite the pressure from Madrid.
Spain's premier is facing the biggest challenge to the constitution in more than three decades as elected officials in Catalonia try to force a rupture with the state.
They refused to move as the day wore on, further angered by an announcement by the interior ministry that police had seized "close to 10 million ballot papers" destined for the vote outlawed by the central government.
Barcelona's national soccer team, FC Barcelona, has released an official statement condemning the acts of the Spanish government against Catalonia.
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Barcelona's mayor Ada Colau tweeted that the raids were a "democratic scandal" and the people of Catalonia would defend their rights.
The Wednesday raids fueled a quick public response on the streets of the Catalan capital. Officials said 80% of them backed independence.
Years of separatist feeling in the industrial northeastern region will come to a head in less than two weeks as the fiercely pro-independence regional government calls a referendum on splitting from Spain.
Pensioner Angel Tena, 63, who had travelled to Barcelona to support the mayor said: 'We consider ourselves privileged to have a mayor who represents the townspeople above any other interests'.
While divided, a large majority of Catalans would like to vote in a legitimate referendum to settle the matter, polls show. But as frictions between Madrid and the Catalan government escalate, sporadic violence and clashes with the police can not be ruled out.
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A survey commissioned by the regional government in July showed that 49.4 percent of Catalans were against independence while 41.1 percent were in favour.
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