Membrane assemblies for electrochemical devices are provided, along with methods and system for fabricating them. Membrane assemblies comprise anode layer(s) and cathode layer(s), separated by membranous separation layer(s) and all embedded in continuous polymerized ionomer material. In production, during continuous deposition of ionomer material on a substrate (e.g., by electrospinning or electrospraying), consecutive deposition stages of catalyst material and optionally binder material are performed. For example, anode particles, binder material and cathode particles may be deposited (e.g., by electrospraying or electrospinning, respectively) consecutively during the continuous deposition o the ionomer material. Self-refueling power-generating system are provided, which include reversible anion exchange membrane devices with disclosed membrane assemblies.