To switch the PayPal account that is linked to Gemini, you will first need to remove the linked PayPal account on the Payment Methods page. You will then be able to add your new PayPal account.
If you would like to change the payment for your Paypal account, you can do so by logging into your PayPal account and navigating to the account settings.
Please note, you are only allowed to link one PayPal account and payment method to your Gemini account at a time. PayPal is only available for customers who reside in the United States.