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Put 1/3 cup sugar and the zest in the bowl of an electric mixer fitted with the paddle attachment. Mix, scraping down the sides of bowl as needed, until combined, about 3 minutes. Set aside. Whisk together flour, baking powder, salt, baking soda, and remaining tablespoon sugar in a medium bowl. Using a pastry blender or two knives, blend in butter until mixture resembles coarse meal. Add buttermilk; stir with a wooden spoon just until a sticky dough forms.
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Turn out dough onto a lightly floured work surface. Pat dough together, and press into an 8-by-11-by-1 inch rectangle. Sprinkle 2 tablespoons sugar mixture on top. Using a bench scraper or spatula to lift dough, fold rectangle into thirds (as you would a letter). Give dough a quarter turn. Roll out into and 8-by-11-by-1 inch rectangle. Sprinkle 2 tablespoons sugar mixture on top. Fold into thirds. Sprinkle remaining sugar on top.
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