Spain, no doubt about it.
I'm not necessarily saying this as an advocate of Basque or Catalan independence. That is a question for the Basque and Catalan people. But a modern, moral, Western country would at least allow a binding referendum, as the UK has done in Scotland and as Canada did in Quebec. If Catalonia has a referendum and they choose to stay part of Spain, that is their choice. But the Spanish government refuses to grant them that choice.
I'm sure EU policy makers on the other hand love small regions becoming independent and wanting to join the EU as they're easier to push around.