How to block internet access for client operating system's DNS over HTTPS
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I think you are on the right track with your With your DoH list on your firewall.
Here are two list i use.https://raw.githubusercontent.com/crypt0rr/public-doh-servers/refs/heads/main/ipv4.list
https://raw.githubusercontent.com/crypt0rr/public-doh-servers/refs/heads/main/ipv6.list
Here is how i have mine set up. go to firewall/aliases/ URLs click add. In properties change the URL type to tables. Add your list.

your update frequency will be stock at 128 days i set mine to 33. Save and then make your firewall rule.

There are more DoH list on github that are more aggressive.
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Thank you @Gertjan for the reply. I will next try to solve the "Unbound python mode" for the next school break.
Thank you @SteveITS for the reply. I was not sure about dns flushing and browser cache issues so what I did was to restart the client PC each time I tested a DoH setting change in the operating system, and pressing shift + [refresh] multiple times on the browser when I typed a URL. The client computer is using pfSense for DNS, DHCP, and internet connection. In case I misunderstood the question this is the services status on the pfSense dashboard:

Thank you @Uglybrian for the suggestion. I have replaced my manual list with your auto-populated list.