A Dual-Bed Catalyst System for Maximizing H2 Production Through Catalytic Partial Oxidation of CH4

The efficient conversion of methane into hydrogen-rich syngas is essential for sustainable energy; however, integrating methane partial oxidation (POM) with the water–gas shift (WGS) reaction remains a significant challenge due to thermal and kinetic mismatches. This research presents a spatially decoupled dual-bed reactor configuration, utilizing Ni/GDC and Cu/GDC catalysts, to achieve synergistic hydrogen production. Unlike conventional physically mixed systems, which suffer from thermal hotspots and the unintended promotion of the endothermic Reverse Water–Gas Shift (RWGS) reaction, the dual-bed architecture effectively segregates the reaction zones. Advanced characterization, including O2-TPO and Raman spectroscopy, reveals that the GDC support acts as a critical oxygen buffer via the Mars-van Krevelen mechanism, modulating the dynamic redox state of the active metal sites to prevent deep oxidation and carbonaceous deactivation. Furthermore, macroscopic performance and carbon–oxygen mass balance analyses confirm that this rational architectural design facilitates a seamless integration of POM and WGS pathways, resulting in significantly maximized H2 yield. From a broader engineering perspective, this dual-bed strategy offers a practical, low-complexity alternative to intensive integrated technologies such as sorption-enhanced reforming (SER) or chemical looping, providing a robust and scalable framework for durable, high-efficiency hydrogen production.