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To find Sync settings, select the Start button, then select Settings > Accounts > Sync your settings. To stop syncing your settings and remove them from the cloud, turn off synced settings on all the devices connected to your Microsoft account, and then go to the Devices page , select More actions for the device you want to manage, and then ...

You can use Windows 10 feature of joining Azure AD domain and then add your PC to the Azure AD domain with your Office 365 subscription. For detailed steps, please see Join a new Windows 10 device with Azure AD during a first run. Here’s a thread for your reference: sign in with Microsoft account instead does not accept office 365.

Thanks for your posting here. Regarding to your problem, I suggest you go to Settings on your PC to disconnect your account and sync again. To do that, please open Start > Settings > Accounts > Access or work school, then disconnect the account in the list.

Hi there, I am signed into a Windows 10 machine with my Office 365 (AzureAD) - (it is a "Workplace or school account") however when I try and enable 'Sync your Settings', I can change it to ON, but then when I click away and come back to this section, it is not saving the change (it is like it does not want to be enabled).

To further isolate the concern, have you verified if the PC's sync settings are actually turned on/off? To check the sync settings, see below: Open Start, and then click on Settings. Click on Accounts. Under Accounts, click on Sync your settings. Check if Sync settings is turned On. If not, click on the switch to turn it on.