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Former U.S. Open runner-up Keys struggled to gain the upper hand in the contest before sealing the opening set in a tiebreak with her eighth ace.
At No. 4, Kenin was the highest-seeded player left in the tournament. She was the runner-up at Roland Garros last October, and was seeking her second major title.
- Kenin showed off her powers of recovery as she racked up a whopping 48 winners and broke Pegula's serve seven times.
Kenin made 18 unforced errors in an unconvincing first-set display but broke decisively in the 11th game as she bagged seven games in a row to open up a 4-0 lead in the second.
Three days earlier, Kenin had admitted to struggling under the pressure of defending her maiden Grand Slam title as she was beaten 6-3 6-2 by Estonian Kaia Kanepi on Margaret Court Arena.