Catalan leader Carles Puigdemont called Monday for worldwide mediation in the crisis pitting his regional separatist executive against Madrid, a day after police violence marred an independence referendum banned by the central government.
In a televised address on Wednesday night, Puigdemont said: "This moment calls for mediation".
Meanwhile, Spain's King Felipe VI said organisers of the vote put themselves "outside the law".
The Catalan health ministry said 893 people were injured in the clashes Sunday as riot police raided polling stations, dragged away voters and fired rubber bullets.
Hundreds of thousands of people across Catalonia have been protesting over Spanish police violence during the vote, during which almost 900 people were hurt, including 33 police officers.
It has been a part of Spain since the 15th century but has a long history of separatist sentiment.
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The Catalan President stopped short of declaring independence from Spain Monday - a move that would further deepen the crisis. The October 1 referendum was an attempt to "break the unity of Spain and national sovereignty, which is the right of all the Spanish people to decide democratically".
Mr. Puigdemont has said that the government of Prime Minister Mariano Rajoy is returning Spain to the authoritarianism of the former dictator, Gen. Francisco Franco.
Carles Puigdemont, the region's elected leader, has asked for European Union mediation in negotiations and said Catalonia has "won the right to an independent state".
Felipe placed the blame for the tension firmly in the hands of the Catalan regional authorities said they "in a repeated, conscious and deliberate manner, have been breaking the Constitution and their Autonomous Status". Demonstrations also took place in several other Catalan cities, including Girona and Lleida.
He said that the use of article 155, and the possible arrest of members of the Catalan government - including himself - could be the "ultimate mistake".
The region's leaders defied Madrid by holding a banned referendum on independence on Sunday.