The free space in LuCI is the free space in the root filesystem overlay.
And it doesn’t make sense to give OpenWrt’s root filesystem overlay more space than what you easily keep in RAM during sysupgrade – it anyway gets reformatted every time you flash an updated firmware.
In order to use the free space on the eMMC for userdata or any other purpose you had in mind I’d recommend you to install uvol and autopart packages. This will allow you to create and manage additional general purpose storage volumes on the eMMC, eg. for userdata or containers or whatever.