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If your flight was cancelled then under article 8 EU Regulation 261/2004 you are entitled to reimburs*m*nt (refund), rescheduling for the earliest date or rescheduling for a date of your choice (subject to conditions).
By reimburs*m*nt the article means:
reimburs*m*nt within seven days, by the means provided for in Article 7(3), of the full cost of the ticket at the price at which it was bought, for the part or parts of the journey not made, and for the part or parts already made if the flight is no longer serving any purpose in relation to the passenger's original travel plan ...
Article 7(3) says of the "means":
cash, by electronic bank transfer, bank orders or bank cheques or, with the signed agreement of the passenger, in travel vouchers and/or other services.
So you are entitled to a cash refund but that doesn't mean you will get one.
It seems some airlines are not informing their customers of their rights and only offering rescheduling or credit vouchers - e.g. TAP - probably to postpone as much of their liability as they can because of the circumstances. And some airlines weren't in a good financial position before this pandemic.
Now, regarding whether the demand should be made of the airline or the agency, with which company do you have a contract? If you don't know, check your bank or card statements. If Expedia charged you then seek a refund from Expedia, if TAP charged you then seek a refund from TAP. The company with which you have a contract is the company that owes you a refund. As Expedia sent you vouchers I guess your contract is with Expedia, but I could be wrong.
So find out which company should refund you, then call them insisting on your right to a refund in cash under Articles 8 and 7. If you are dissatisfied with their response try a chargeback.
(Perhaps interesting to note it's in your individual interest to do that but it is not in yours or everyone's interest for everyone to do that.)
If you can't get a refund, if you have travel insurance and can persuade the insurer the money is not recoverable then the insurer may cover it - check your policy. If you haven't bought travel insurance it's worth looking into whether your bank(s) provided a policy 'free' with your account.
Those are things you can do in the short-term.
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It's definitely difficult situation. The way I see it you have these options:
Do you have travel insurance?
You're entitled to a refund but it will be difficult to get it
Try to claim it from American Express (Section 75 Refunds)