Ctrl and Alt can be used. In certain contexts they will be problematic, because they have hard coded functions related to brush behavior. When you fully understand these behaviors, you’ll get a sense for when and why there might be a conflict.
For instance, [Ctrl +; ] works perfectly fine as a shortcut for the Delete Loops function. As does [Shift + ; ], as does [Shift + Ctrl + ; ], as does [Shift + Ctrl + Alt + ; ].
You just have to understand that those keys toggle ongoing effects related to brushes, and if you try to assign them also to another ongoing effect or brush related effect to be used while brushing, there are likely to be conflicts. For instance Shift will always activate smooth mode, which will result in any changes to the active brush being applied to the smoothing brush. If you try to use shift to activate some other feature related to the active sculpting brush, it is likely to cause problems.
If you’d like to request more hotkey opportunities, that request needs to be submitted to Pixologic Support. This is just the community forum. We don’t develop the program.