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One of the original proposals for the UN headquarters was on Navy Island near Niagara Falls. The proposal was made in 1945 and had some interesting points in it. The headquarters was to encompass the entire island putting it on a national border, and Canada agreed to cede the island to the United Nations while it remained there. Would the location, especially with the UN having sovereign territory, change much? Could the UN being on sovereign territory make it be perceived as more neutral, and thus maybe be more effective?
Also, here is a picture of the proposed site (warning: big image). Looks quite nice IMO.