If you cannot pair your controllers or cannot pair a second controller, the tips listed below might be able to help you. Make sure the controllers are charged. When something abnormal happens to your controller, this is the first thing you should try. Unpair the controller, reboot SteamVR and pair again. Update the firmware using USB 2.0 port instead of USB 3.0. Clear other wireless devices like TV remotes, cell phones from the play area. They might be interrupting. Reset the controller. Hold down everything except the system button and plug the controller into PC via USB cable. Wait for 5 seconds and release the buttons. Then just unplug it from the PC. Uninstall and install SteamVR and restart the PC.
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