Intermittent freezing (including in BIOS) - I built my daughter a gaming PC (Z690, Intel i9, GeForce RTX 3080) was fine for a year, no changes made.

Lot of paste squashed out the side
Not quite enough in the middle really
Though have seen worse
If unsure how much to use
Or how to apply it
Ie a blob or a x etc
I suggest use an old credit card/bit of cardboard etc
And spread a thin even coating on

Would have to go read all the previous posts
But if AIO need to be sure pumps running
Mine hit 80c+ very fast
When I first installed it the pump defaulted to 300rpm
For some reason
I had to jump straight in the bios
And find fan control and hit a preset like normal/fast/turbo etc

Upgrading the psu while may not
Have fixed it
Is still not a total waste of money
A good psu will last you a long time
 
As long as the CPU block is on properly, the most likely thing that could cause those temps is an airlock or failed pump in the AIO.

Double check the pump to MB header connection to ensure it's still connected. If you've reset the BIOS recently, ensure the header is still in WaterPump/Continuous mode. The BIOS sensor page should show you the pump speed.

With the pump in the orientation you have now, its possible you have an air bubble stuck in the block. To remove it, take out the rad, invert the case and hold the rad above the cpu block while the system is running so that any bubbles rise into the rad. If it has a top up port, top it up first.

With all the strange behaviour I think it's looking likely it's a motherboard issue.
 
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So an update, it’s been a while partially due to a mix of buyers remorse and procrastination! Full disclosure - I induced the CPU overheating fault by plugging the AIO cable that connects to the pump in backwards. Idiot, luckily it didn’t do any damage.

Anyway, it hasn’t frozen yet, I’ll get my daughter to stress it with some games this evening to test properly.

Things I did (thanks everyone for the advice):
- redid the heat sink paste evenly with a more reasonable amount (IE less).
- made half the fans intake and half exhaust.
- plugged the radiator fans directly into the CPU fan header on the motherboard rather than the Lian-Li control box.
- added an internal USB hub (SATA powered) as there weren’t enough headers on the motherboard for the Corsair control box, the Lian-Li control box and the Kracken AIO cooler.
- Replaced the 750W Corsair power supply with a 1000W ASUS one.
 
So, it seems to have been fixed the cpu remount, and then actually connecting the pump correctly? Shame about an extra psu, but at least you've got a spare, or can always sell it on :)
 
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