The authentication flow supported with Barclays uses the following credentials:

Last name
Membership number
Memorable word

If you are trying to use Pinsentry, we don't support this, not even to generate the Passcode. You need to set Passcode and Memorable word via online banking and use these credentials.

Where can I set Passcode and Memorable word?

These can be set online on the Barclays website. There is a section in Personal details that lets you do so.

After you have set them, make sure to test them via the Barclays website first.
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