I am not sure if The Home For The Friendless was on Peachtree, but it is possible. My Grandpa Willard Snow and his sister Maude Snow were in it somewhere between 1900 and 1910. It burned in a fire and there are only two journals that survived which are housed at Emory University, Rare Collections. I could not find my Grandpa's name or his sister's.
My Grandpa took my father there once after it burned to show him where it was located, but I do not know the name of the street, but I do know it was in Downtown Atlanta.
If this could be it, I have a write up about the Orphanage from a newspaper. Email me at firstname.lastname@example.org
for more on the article.