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No, this should not be done. The VOS pin must be connected directly at the output cap near the IC.
In addition, the VOS pin is not responsible for the DC setpoint. This is accomplished through the FB pin.
It may be possible to connect the high side of the upper FB resistor to your load, but for a 1A device like the TPS62080, I don't think you compensate for very much IR drop.
Instead, I would recommend the TPS62360 family, which has true differential remote sense and a tighter output voltage accuracy.
Yes, you can ground those pins if you don't need I2C. You can still change the output voltage among the 4 presets with the VSELx pins.