Something already proposed for that block: (east of the gas station)
https://www.gordperks.ca/nov_9_23 Community Meeting to discuss development proposal at 1730 Bloor Street West The property owners of 1730 Bloor St West, current site of strip mall and 7-11, is holding an Online Community Meeting to share preliminary plans for a 25-storey mixed-use development...
urbantoronto.ca
Even if you get the entire block, all that buys you is platform width, it doesn't get you additional bus bays, which is what is needed there.
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If you kept the bus terminal roughly where it is today, you could buy 4 or so properties to the north and stagger the bus bays in a saw-tooth pattern, that would get you 1 additional bus bay (north side only)
Fairly expensive relative to the pay off. An alternative choice, providing that it can be graded to deal w/any flooding issues is to the move the bus platform to the eastern 1/2 of the station, east of Indian Grove. (currently parking)
That would allow roughly 4 additional bus bays (including replacing the existing ones)
The challenge is the limited space for access off the east end of the Keele Platform; and you would need another set of elevators.
On top of that, the buses would all have to enter/exit via Indian Road, and Bloor, which would be a bit of a pain.
View attachment 520999
There is one other alternative, I suppose, but I don't think it would impress the locals:
View attachment 521000
The bus platform could be extended out to the TTC property limit and the buses could circle using Indian Grove.
This wouldn't necessarily result in the closure of Indian Grove at Bloor; though that would be be an option, but it would be congested w/all those buses if you didn't.
That extension would get you 2 additional bus bays at the existing station. (one on the north, one on the south)