@Catherine250
They may be used to hotel 24/7 service. You'll have to put on your big-Girl pants and confront them that this is not suitable behaviour.
(Remember to recap any off-site conversation on the message page as proof in case later required).
They are endangering your property when not being careful with the keys and you can use that wording. They're also not being considerate to a host in a shared space, so enough reason to tidy up their act.
But like it or not, you'll have to confront them, unless they're only staying for a few days. You've actually already waited a day too long. Always better to not wait too long. "Hey guys, this isn't working so well, we need to talk about ..."
Your house, your rules.
If they are staying longer and don't make an effort, remind them again (and recap in message system) and you can ask them if they'd rather be relocated by Airbnb to another accommodation better suited for their needs. That apparently has gotten many a guest wizened up quickly when they see you're not a doormat.
Review: "Guests were friendly [or whatever, blabla] but seem better suited to commercial and non-shared rentals."
Then give them a thumbs down.
Hosting - being tough as steel with a friendly face.