In a televised address, King Felipe said the Catalan leaders had "infringed the system of legally approved rules with their decisions, showing an unacceptable disloyalty towards the powers of the state".
In spite of controversy and violence that surrounded Sunday's referendum for Catalonia, leader Carles Puigdemont says the Spanish region has won the right to statehood.
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Spain's interior minister said the 5,000 extra officers would stay in Catalonia as long as necessary.
The tensions in Catalonia, Spain's northeastern region, are mounting.
Puigdemont warned that if the Spanish government attempted to intervene and take control of Catalonia's government, it would be "an error which changes everything".
The National Court in Madrid summoned Josep Luis Trapero and three other suspects to a hearing on Friday, said the spokesman, who asked not to be named.
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The reigning Spanish monarch said the referendum had shown a "lack of loyalty" to the government, criticising the referendum as undemocratic.
The people were attacked by the police when trying to vote on the referendum. These are very complex moments, but we will move forward.
"I urge the Spanish authorities to ensure thorough, independent and impartial investigations into all acts of violence", he said, stressing, "Police responses must at all times be proportionate and necessary".
"There are people who interpret the Constitution like the Bible, like it contains absolute truths, that it's more important than the will of the people", the Catalonian leader said.
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The Catalan government has called on the global community - the European Union in particular - to mediate. Most of San Rafael, including the town hall, is in the Valencia region, which has no plans to leave Spain.
Several high-ranking officials were subjected to a series of recent early morning raids by national police, in a bid to prevent the vote from happening.
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