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If you have mounted that share from the server to your client (ie where you are logged in) then you can't umount it if any process at all is using that mount, including if your current working dir (pwd) ie where you are, is on that mount. You have to cd elsewhere.
Otherwise check lsof, fuser.
after you've done the manual mount. You can pretty much cut 'n paste the relevant line into /etc/fstab.
The system knows how to mount stuff, that's why the manual cmd is different, the system only needs to be told what to mount, where and any options.
PS do NOT edit /etc/mtab(!)