Config for running Unbound as a caching DNS forwarder (performance settings optimized for Raspberry Pi 2).

unbound.conf

server:
    ###########################################################################
    # BASIC SETTINGS
    ###########################################################################
    # Time to live maximum for RRsets and messages in the cache. If the maximum
    # kicks in, responses to clients still get decrementing TTLs based on the
    # original (larger) values. When the internal TTL expires, the cache item
    # has expired. Can be set lower to force the resolver to query for data
    # often, and not trust (very large) TTL values.
    cache-max-ttl: 86400

    # Time to live minimum for RRsets and messages in the cache. If the minimum
    # kicks in, the data is cached for longer than the domain owner intended,
    # and thus less queries are made to look up the data. Zero makes sure the
    # data in the cache is as the domain owner intended, higher values,
    # especially more than an hour or so, can lead to trouble as the data in
    # the cache does not match up with the actual data any more.
    cache-min-ttl: 300

    # Set the working directory for the program.
    directory: "/opt/unbound/etc/unbound"

    # RFC 6891. Number of bytes size to advertise as the EDNS reassembly buffer
    # size. This is the value put into datagrams over UDP towards peers.
    # 4096 is RFC recommended. 1472 has a reasonable chance to fit within a
    # single Ethernet frame, thus lessing the chance of fragmentation
    # reassembly problems (usually seen as timeouts). Setting to 512 bypasses
    # even the most stringent path MTU problems, but is not recommended since
    # the amount of TCP fallback generated is excessive.
    edns-buffer-size: 1472

    # Listen to for queries from clients and answer from this network interface
    # and port.
    interface: 0.0.0.0@53

    # Rotates RRSet order in response (the pseudo-random number is taken from
    # the query ID, for speed and thread safety).
    rrset-roundrobin: yes

    # Drop user  privileges after  binding the port.
    username: "_unbound"

    ###########################################################################
    # LOGGING
    ###########################################################################

    # Do not print log lines to inform about local zone actions
    log-local-actions: no

    # Do not print one line per query to the log
    log-queries: no

    # Do not print one line per reply to the log
    log-replies: no

    # Do not print log lines that say why queries return SERVFAIL to clients
    log-servfail: no

    # Further limit logging
    logfile: /dev/null

    # Only log errors
    verbosity: 0

    ###########################################################################
    # PRIVACY SETTINGS
    ###########################################################################

    # RFC 8198. Use the DNSSEC NSEC chain to synthesize NXDO-MAIN and other
    # denials, using information from previous NXDO-MAINs answers. In other
    # words, use cached NSEC records to generate negative answers within a
    # range and positive answers from wildcards. This increases performance,
    # decreases latency and resource utilization on both authoritative and
    # recursive servers, and increases privacy. Also, it may help increase
    # resilience to certain DoS attacks in some circumstances.
    aggressive-nsec: yes

    # Extra delay for timeouted UDP ports before they are closed, in msec.
    # This prevents very delayed answer packets from the upstream (recursive)
    # servers from bouncing against closed ports and setting off all sort of
    # close-port counters, with eg. 1500 msec. When timeouts happen you need
    # extra sockets, it checks the ID and remote IP of packets, and unwanted
    # packets are added to the unwanted packet counter.
    delay-close: 10000

    # Prevent the unbound server from forking into the background as a daemon
    do-daemonize: no

    # Add localhost to the do-not-query-address list.
    do-not-query-localhost: no

    # Number  of  bytes size of the aggressive negative cache.
    neg-cache-size: 4M

    # Send minimum amount of information to upstream servers to enhance
    # privacy (best privacy).
    qname-minimisation: yes

    ###########################################################################
    # SECURITY SETTINGS
    ###########################################################################
    # Only give access to recursion clients from LAN IPs
    access-control: 127.0.0.1/32 allow
    access-control: 192.168.0.0/16 allow
    access-control: 172.16.0.0/12 allow
    access-control: 10.0.0.0/8 allow
    # access-control: fc00::/7 allow
    # access-control: ::1/128 allow

    # File with trust anchor for  one  zone, which is tracked with RFC5011
    # probes.
    auto-trust-anchor-file: "var/root.key"

    # Enable chroot (i.e, change apparent root directory for the current
    # running process and its children)
    chroot: "/opt/unbound/etc/unbound"
    
    # Deny queries of type ANY with an empty response.
    deny-any: yes

    # Harden against algorithm downgrade when multiple algorithms are
    # advertised in the DS record.
    harden-algo-downgrade: yes

    # RFC 8020. returns nxdomain to queries for a name below another name that
    # is already known to be nxdomain.
    harden-below-nxdomain: yes

    # Require DNSSEC data for trust-anchored zones, if such data is absent, the
    # zone becomes bogus. If turned off you run the risk of a downgrade attack
    # that disables security for a zone.
    harden-dnssec-stripped: yes

    # Only trust glue if it is within the servers authority.
    harden-glue: yes

    # Ignore very large queries.
    harden-large-queries: yes

    # Perform additional queries for infrastructure data to harden the referral
    # path. Validates the replies if trust anchors are configured and the zones
    # are signed. This enforces DNSSEC validation on nameserver NS sets and the
    # nameserver addresses that are encountered on the referral path to the 
    # answer. Experimental option.
    harden-referral-path: no

    # Ignore very small EDNS buffer sizes from queries.
    harden-short-bufsize: yes

    # Refuse id.server and hostname.bind queries
    hide-identity: yes

    # Refuse version.server and version.bind queries
    hide-version: yes

    # Report this identity rather than the hostname of the server.
    identity: "DNS"

    # These private network addresses are not allowed to be returned for public
    # internet names. Any  occurrence of such addresses are removed from DNS
    # answers. Additionally, the DNSSEC validator may mark the  answers  bogus.
    # This  protects  against DNS  Rebinding
    private-address: 10.0.0.0/8
    private-address: 172.16.0.0/12
    private-address: 192.168.0.0/16
    private-address: 169.254.0.0/16
    # private-address: fd00::/8
    # private-address: fe80::/10
    # private-address: ::ffff:0:0/96

    # Enable ratelimiting of queries (per second) sent to nameserver for
    # performing recursion. More queries are turned away with an error
    # (servfail). This stops recursive floods (e.g., random query names), but
    # not spoofed reflection floods. Cached responses are not rate limited by
    # this setting. Experimental option.
    ratelimit: 1000

    # Use this certificate bundle for authenticating connections made to
    # outside peers (e.g., auth-zone urls, DNS over TLS connections).
    tls-cert-bundle: /etc/ssl/certs/ca-certificates.crt

    # Set the total number of unwanted replies to eep track of in every thread.
    # When it reaches the threshold, a defensive action of clearing the rrset
    # and message caches is taken, hopefully flushing away any poison.
    # Unbound suggests a value of 10 million.
    unwanted-reply-threshold: 10000

    # Use 0x20-encoded random bits in the query to foil spoof attempts. This
    # perturbs the lowercase and uppercase of query names sent to authority
    # servers and checks if the reply still has the correct casing.
    # This feature is an experimental implementation of draft dns-0x20.
    # Experimental option.
    use-caps-for-id: yes

    # Help protect users that rely on this validator for authentication from
    # potentially bad data in the additional section. Instruct the validator to
    # remove data from the additional section of secure messages that are not
    # signed properly. Messages that are insecure, bogus, indeterminate or
    # unchecked are not affected.
    val-clean-additional: yes

    ###########################################################################
    # PERFORMANCE SETTINGS
    ###########################################################################
    # https://nlnetlabs.nl/documentation/unbound/howto-optimise/

    # Number of slabs in the infrastructure cache. Slabs reduce lock contention
    # by threads. Must be set to a power of 2.
    infra-cache-slabs: 4

    # Number of slabs in the key cache. Slabs reduce lock contention by
    # threads. Must be set to a power of 2. Setting (close) to the number
    # of cpus is a reasonable guess.
    key-cache-slabs: 4

    # Number  of  bytes  size  of  the  message  cache.
    # Unbound recommendation is to Use roughly twice as much rrset cache memory
    # as you use msg cache memory.
    msg-cache-size: 128525653

    # Number of slabs in the message cache. Slabs reduce lock contention by
    # threads. Must be set to a power of 2. Setting (close) to the number of
    # cpus is a reasonable guess.
    msg-cache-slabs: 4

    # The number of queries that every thread will service simultaneously. If
    # more queries arrive that need servicing, and no queries can be jostled
    # out (see jostle-timeout), then the queries are dropped.
    # This is best set at half the number of the outgoing-range.
    # This Unbound instance was compiled with libevent so it can efficiently
    # use more than 1024 file descriptors.
    num-queries-per-thread: 4096

    # The number of threads to create to serve clients.
    # This is set dynamically at run time to effectively use available CPUs
    # resources
    num-threads: 3

    # Number of ports to open. This number of file descriptors can be opened
    # per thread.
    # This Unbound instance was compiled with libevent so it can efficiently
    # use more than 1024 file descriptors.
    outgoing-range: 8192

    # Number of bytes size of the RRset cache.
    # Use roughly twice as much rrset cache memory as msg cache memory
    rrset-cache-size: 257051306

    # Number of slabs in the RRset cache. Slabs reduce lock contention by
    # threads. Must be set to a power of 2.
    rrset-cache-slabs: 4

    # Do no insert authority/additional sections into response messages when
    # those sections are not required. This reduces response size
    # significantly, and may avoid TCP fallback for some responses. This may
    # cause a slight speedup.
    minimal-responses: yes

    # # Fetch the DNSKEYs earlier in the validation process, when a DS record
    # is encountered. This lowers the latency of requests at the expense of
    # little more CPU usage.
    prefetch: yes

    # Fetch the DNSKEYs earlier in the validation process, when a DS record is
    # encountered. This lowers the latency of requests at the expense of little
    # more CPU usage.
    prefetch-key: yes

    # Have unbound attempt to serve old responses from cache with a TTL of 0 in
    # the response without waiting for the actual resolution to finish. The
    # actual resolution answer ends up in the cache later on.
    serve-expired: yes

    # Open dedicated listening sockets for incoming queries for each thread and
    # try to set the SO_REUSEPORT socket option on each socket. May distribute
    # incoming queries to threads more evenly.
    so-reuseport: yes

    ###########################################################################
    # LOCAL ZONE
    ###########################################################################

    # Include file for local-data and local-data-ptr
    include: /opt/unbound/etc/unbound/a-records.conf

    ###########################################################################
    # FORWARD ZONE
    ###########################################################################
    forward-zone:
        # Forward all queries (except those in cache and local zone) to
        # upstream recursive servers
        name: "."
        # Queries to this forward zone use TLS
        forward-tls-upstream: yes

        # https://dnsprivacy.org/wiki/display/DP/DNS+Privacy+Test+Servers

        # Cloudflare
        forward-addr: 1.1.1.1@853#cloudflare-dns.com
        forward-addr: 1.0.0.1@853#cloudflare-dns.com
        #forward-addr: 2606:4700:4700::1111@853#cloudflare-dns.com
        #forward-addr: 2606:4700:4700::1001@853#cloudflare-dns.com

        # CleanBrowsing
        forward-addr: 185.228.168.9@853#security-filter-dns.cleanbrowsing.org
        forward-addr: 185.228.169.9@853#security-filter-dns.cleanbrowsing.org
        # forward-addr: 2a0d:2a00:1::2@853#security-filter-dns.cleanbrowsing.org
        # forward-addr: 2a0d:2a00:2::2@853#security-filter-dns.cleanbrowsing.org

        # Quad9
        # forward-addr: 9.9.9.9@853#dns.quad9.net
        # forward-addr: 149.112.112.112@853#dns.quad9.net
        # forward-addr: 2620:fe::fe@853#dns.quad9.net
        # forward-addr: 2620:fe::9@853#dns.quad9.net

        # getdnsapi.net
        # forward-addr: 185.49.141.37@853#getdnsapi.net
        # forward-addr: 2a04:b900:0:100::37@853#getdnsapi.net

        # Surfnet
        # forward-addr: 145.100.185.15@853#dnsovertls.sinodun.com
        # forward-addr: 145.100.185.16@853#dnsovertls1.sinodun.com
        # forward-addr: 2001:610:1:40ba:145:100:185:15@853#dnsovertls.sinodun.com
        # forward-addr: 2001:610:1:40ba:145:100:185:16@853#dnsovertls1.sinodun.com

remote-control:
    control-enable: no

The device was actually off for over 24 hours

That's what triggers the issue, since RPi system clocks starts where it left off at shutdown in the next power-on.

To my knowledge this is caused by dnssec so if you are ok with disabling that go for it. Personally as someone who uses it 24/7 with minor down time if an sd card fails or i meed to update then it works just fine.

In case of unmanned and remotely inaccessible RPi with no local time server available, one can consider adding this option to allow time sync and then using DNSSEC still after time is correct:

server:
    val-permissive-mode: yes

See also https://nlnetlabs.nl/documentation/unbound/howto-turnoff-dnssec