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Methods of making an environmental barrier coating (EBC) for a substrate are provided that include providing an EBC feedstock comprising a rare earth element composition, in which a portion of the composition produces a volatile species during an air plasma spray coating process, providing a first additive that comprises or produces the volatile species during the air plasma spray coating process, injecting the EBC feedstock into a plasma spray plume during the air plasma spray coating process; and injecting the first additive into at least one of the plasma spray plume and a plasma torch nozzle during the air plasma spray coating process, in which the EBC has a composition that is substantially similar to the composition of the EBC feedstock.