Enhanced Hydrogen Production in Microwave‐Driven Water‐Splitting Redox Cycles by Engineering Ceria Properties

Abstract

AbstractSustainable hydrogen, produced from renewable sources such as solar or wind, plays a decisive role in driving industrial decarbonization. Among hydrogen production technologies, steam electrolysis, and solar‐driven thermochemical cycles using reducible solid oxides show promise but face challenges due to high operation temperatures. Microwave‐driven redox chemical looping enables the direct, contactless electrification of the process, reducing the operation temperature and complexity. Previous works showed that microwaves can efficiently drive reduction/water‐splitting cycles using Gd‐doped ceria at low temperatures (<250 °C), but adjustment of material properties is needed. Here, the key properties of materials are explored that affect the redox mechanism by screening a series of doped ceria materials to enhance microwave‐driven hydrogen production. Evaluation of trivalent dopants (La3+, Gd3+, Y3+, Yb3+, Er3+, and Nd3+) reveals that reduction correlates with lattice and electronic properties. The composition Ce0.9La0.1O2‐δ achieves 1.41 mL g−1, the highest hydrogen production among the studied series. Its narrower bandgap allows for reaching higher conductivity upon microwave‐driven reduction at lower temperatures, while a larger ionic lattice size boosts solid‐state oxygen diffusion. Overall, this research remarks on the critical properties of ceria‐based materials that enhance hydrogen production in microwave‐driven water‐splitting cycles, supporting the design of more efficient materials for sustainable chemical production technology.