An Integrated Hydrogen Cascade Reactor for Formic Acid Dehydrogenation, Membrane Purification, and On‐Demand Hydrogenation

We report an integrated hydrogen cascade reactor that couples formic acid dehydrogenation, selective H 2 separation, and downstream hydrogenation within a single system. A redox‐active bimetallic PdNi‐chloranilate (PdNiCA) metal–organic framework (MOF) catalyst enabled H 2 generation from formic acid under mild conditions, while a mixed‐conducting graphene oxide membrane selectively transported hydrogen and effectively suppressed CO 2 permeation. The separated H 2 was directly supplied to a downstream reaction chamber without intermediate storage or external purification and used for nitroarene hydrogenation under ambient conditions. Representative nitroarenes were converted to the corresponding anilines with conversions of up to 99%, demonstrating that the membrane‐delivered hydrogen was sufficiently reactive for downstream chemical transformation. By integrating H 2 production, purification, and utilization within a single architecture, this system offers a low‐temperature strategy for on‐demand hydrogen utilization and highlights the potential of membrane‐integrated reactors for sustainable hydrogen‐driven synthesis.