Catalan government spokesman Jordi Turull said Spain had become "the shame of Europe" after scenes of police taking on voters were beamed around the world and splashed across the front pages.
The region's largest opposition party mounted a legal challenge and filed a writ of protection with the federal tribunal, saying that a declaration of independence by Catalonia would violate the constitution and "destroy" the rights of regional deputies, according to El Pais newspaper on Thursday.
Catalonia's president has called for further mediation to tackle the region's secession crisis and accused King Felipe VI of acting as a mouthpiece for the Spanish government and of "deliberately ignoring millions of Catalans".
Accusing them of "disloyalty", the king said that the state had to "ensure constitutional order".
The organisers said 90 per cent voted for independence, but have not published the final results.
"The threats of separatism do not scare us", said Xavier Garcia Albiol, the head of the ruling Popular Party in Catalonia, on Tuesday, as around 2,000 people surrounded party headquarters.
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Barcelona Mayor Ada Colau called on European institutions to consider setting up a task force of experts to mediate after meeting consular representatives of European countries.
Two million Catalans voted in favour of the region breaking away from Spain and forming an independent republic in Sunday's referendum of independence, which saw a turnout of about 40 per cent.
"If somebody tries to declare the independence of part of the territory - something that can not be done - we will have to do everything possible to apply the law", Catalá said.
"[A suspension of Catalonia's autonomy] will be another error in a long list of mistakes".
Likewise, the utter lack of dialogue between the governments in Madrid and Barcelona remains.
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There are several reports of gaping irregularities, partly attributed to a system which permitted voters to cast their ballots anywhere in a bid to get around the police measures to stop the vote.
Guadalupe Espinosa, a 47-year-old psychologist who lives on the Catalan side of the river, said: "People are nervous and scared because they feel this is a free-fall".
That would further enrage Catalan protesters, who say they are being repressed by Spain.
Most of San Rafael, including the town hall, is in the Valencia region, which has no plans to leave Spain.
About 200 people gathered in front of Spanish government buildings and chanted " You are not alone" and "This is our police" to the officers from the Spanish National Police and Guardia Civil who guard the buildings. As anticipation of a U.S. rate increase spread to more than 71 percent by December from 42 percent a month earlier, according to the CME's Fedwatch indicator, the dollar has rallied more than 3 percent over the last month.
The Catalan government has called on the global community - the European Union in particular - to mediate.
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