Ironically, the Catalan government has suggested that the European Union could be a mediator in its negotiations with Madrid.
According to a bill passed by the Catalan parliament in September, the region will declare independence from Spain within 48 hours of a Yes vote.
He says "this is an internal matter for Spain that has to be dealt with in line with the constitutional order of Spain". Catalans came out on to the streets on Tuesday to condemn the police action, shutting down road traffic, public transport and businesses, and ratcheting up fears of intensifying unrest in a region that makes up one-fifth of the Spanish economy.
Speaking in the European Parliament on Wednesday, the top eurocrat condemned Catalonia's regional government for holding a vote on independence, saying it had "chosen to ignore the law in organising the referendum of last Sunday", Politico reports. The vote did not have any census controls, electoral board or official vote-counting teams or worldwide observers of any weight.
Police seized ballot boxes, pulled people out of polling stations and fired rubber bullets at protesters - with hundreds reportedly injured.
"With this speech, the king opens the door to all measures included in the Constitution to restore constitutional order", said Fermin Urbiola, the author of books on the Spanish monarchy and other European royal families.
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It is thought many who oppose independence simply stayed away - but Mr Mas insisted that, given the circumstances surrounding the election, the turnout was encouraging.
Provisional results of the referendum that the Spanish government considers illegal showed the "Yes" side winning 90 percent of the 2.3 million votes cast, which is less than half the region's electorate.
Catalan President Carles Puigdemont also wants the European Union to trigger a mechanism known as Article 7 which would suspend the membership rights of Spain on the grounds that it has breached European Union values like the respect for human rights or the rule of law. Spain cried foul and most governments backed it.
"Valencia and Catalonia are different, but even though the border exists, it's the same town", 20-year-old lifeguard Natzari Reverte said. But that could change Monday if Puigdemont and his supporters have their way. The regional leader of Catalonia has offered talks with Madrid to resolve the crisis.
Spain has been thrown into turmoil in these past few days; brother turned against brother, state against country. The region of Catalonia is shown in red. The new Catalan state would also already be in debt, as Madrid and Barcelona would have to determine what percentage of Spain's sovereign debt Catalonia would inherit. Whatever leverage it once had in mediating conflicts in countries such as Colombia and Guatemala could be lost.
"The EU must and should be this third party in talks".