Pi-Hole appears to be configured correctly, but does not block ads

Below some hints:

DHCP is IPv4 only.
DHCPv6 exists but isn't supported on a bunch of OS'es like Android.
IPv6 RA (Router Advertisement) is the way to advertise IPv6 DNS IP's to your clients:

https://www.rfc-editor.org/rfc/rfc8106

If you install below on the Raspi, you can inspect what is advertised on your LAN and from which MAC address the RA is coming from:

Example outputs in that same thread.

The official docs have a "Router setup" section that also includes TP-Link: