This invention provides new and novel devices and methods for administering lithium (Li) ions to a mammalian subject, especially the delivery of lithium (Li) ions to a body component for example across a body or tissue surface such as skin or a mucosal membrane, or for delivery of lithium ions directly to bodily fluids in a controllable and reproducible manner. In certain embodiments the device comprises a donor electrode that is a donor of a lithium ion; a protective architecture that is ionically conductive to the lithium ion, configured for application to a skin surface and positioned to isolate said donor electrode from the skin surface; and a counter electrode assembly configured for application to a skin surface, where said counter electrode assembly comprises a counter electrode operably coupled to said donor electrode.