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Mertens transferred to PSV Eindhoven in 2011. He had previously played for AGOVV Apeldoorn and FC Utrecht in the Netherlands. Mertens quickly established himself as a key player for PSV, scoring 37 goals in 92 appearances for the club. He helped PSV win the Eredivisie title in 2012 and 2015, and the KNVB Cup in 2012.