Yes, you can, but only if you want to set up as self employed Autonomo, either as start capital or to fund your Autonomo contributions.
When can you ask for the single payment?
The self-employment activities for which the single payment of unemployment can be requested are:
The beginning of an activity as a self-employed worker.
The incorporation into a cooperative, existing or newly created, as a working or stable working partner.
The constitution of a labor society or the incorporation of an existing one, as a working or stable working partner.
The creation of a newly established commercial entity (for example an SL) or joining one that has been created in the previous 12 months, if you are going to have control of it.