Wireless Electrochemical Palladium Membrane Reactor

Abstract

Electrochemical palladium membrane reactors traditionally rely on direct cathodic polarization of the palladium membrane to drive hydrogen permeation. This work introduces the wireless electrochemical palladium membrane reactor (wPMR), a design that utilizes bipolar electrochemistry to actuate hydrogen transport without direct electrical connections to the membrane. By redefining the palladium membrane as an “ajar” bipolar electrode, we demonstrate that it functions similarly to a diode, requiring a voltage threshold to initiate selective hydrogen transport along an induced external electric field. As a proof-of-concept, we integrated the wPMR with lithium-mediated nitrogen reduction, successfully synthesizing ammonia using hydrogen atoms derived directly from water. Unlike conventional systems that suffer from structural deformation due to lattice expansion, the wPMR maintains membrane integrity by avoiding the lattice-expanded β-PdH. Through isotope labeling and operando monitoring, we confirm the synchronous operation of four Faradaic reactions within this reaction geometry. The wPMR thus emerges as a high-voltage electrosynthetic platform capable of directly delivering hydrogen from water to organic reactions.