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If that don't work empty the account of its money. That'll stop all the payments for sure.
Of course you could make a Steam Support ticket, get annoyed at the autoresponder answering something completely different, asking again and then they can maybe handle it but only have it effective by the date of the support ticket. Don't provide card info until they ask.
https://help.steampowered.com/en/faqs/view/726E-E811-168F-0D9E
When adding a subscription to the cart, you should be able to select a different payment type by going back one step during the checkout process if you have a default payment method already set up. (It's something I do fairly often with normal purchases, in fact.)