I don’t believe it is possible to tell if a given number is in service or not without contact the credit card company. Mockaroo simply generates numbers that are valid according for the formulas described here: https://en.wikipedia.org/wiki/Payment_card_number. I think the only way to ensure a number is not in use to to make it invalid. You can do this using the inline formula feature (the f(x) button) to change the generated value to your liking.
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