The EPA issued the two air quality permits last year, allowing Shell to operate a drilling ship and support vessels in the area.
But an appeal brought by conservation and indigenous groups, which claimed the EPA had applied outdated nitrogen dioxide standards, was upheld by the EPA Environmental Appeals Board.
When awarded, the permits complied with national ambient air quality standards for nitrogen dioxide, but a later decision found those standards did not provide sufficient protection.
The board decision will require the permits to be renegotiated between Shell and the EPA.
Alaska Governor Sean Parnell said he was disappointed by the decision, which he said came after a series of delays.
"Nothing can replace the jobs that Alaska and America lose when one resource project after another is delayed by endless appeals,” he said.
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