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I would recommend looking at these
http://community.us.playstation.com/t5/PlayStation-3/Playstation-3-will-not-sync-any-controllers-Help/td-p/31035411
http://community.us.playstation.com/t5/Support-General/Controllers-will-not-sync-up/td-p/37040568
http://community.us.playstation.com/t5/PlayStation-3/Controller-not-syncing-with-PS3/td-p/17195345
Well, this little trick always works. Turn your controller to the back side and you'll see to the left of the L2 button a small hole. Switch on your controller and put a pin inside the hole and hold it there for 5 seconds. This is the reset button. The controller should connect now when you switch it on again.
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