Hi Christopher,
You cannot increase quota on Azure Free account. You must first upgrade to Pay-As-You-Go account if you want to request quota increase. Below is excerpt from documentation:
...Free subscriptions including Azure Free Account and Azure for Students aren't eligible for limit or quota increases. If you have a free subscription, you can upgrade to a Pay-As-You-Go subscription.
Please click Accept Answer and upvote if the above was helpful.
Thanks.
-TP