Catalonia's leader Artur Mas reached out to Madrid for talks on a "definitive" and binding vote, but the national government, which had tried to ban Sunday's ballot, dug in its heels.
"The right to self-determination is not possible, neither under our constitution nor in any of the other democracies around us," Deputy Prime Minister Soraya Saenz de Santamaria told parliament.
Demands for greater autonomy for the rich northeastern region have grown over recent years, fanned by Madrid's resistance and the recent economic crisis.
Mas said he had written to Prime Minister Mariano Rajoy on today inviting him "to set the conditions for a dialogue that is permanent and as constructive as possible".
The ultimate aim is to hold "a definitive and politically binding consultation" vote, Mas added.
Rajoy fiercely opposed Sunday's symbolic vote and has not reacted since the polls, in which 1.86 million people voted for independence.
Mas had hoped the vote would strengthen his hand in trying to force concessions from Rajoy, who has vowed to defend the unity of Spain as it recovers from recession.
"If what you want is independence for Catalonia, it will be difficult for us to come to an agreement," the deputy prime minister told the upper house Senate.
"Neither this party nor this government will vote for an agreement on secession."
The dispute looked set to drag on.
Mas did not rule out calling a snap regional election to be fought exclusively on the independence issue.
He said he would hold talks over the coming weeks with other Catalan political parties to gauge support for such a move.
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