Tunning Pd-Cu-based catalytic oxygen carrier for intensifying low-temperature methanol reforming

Methanol is a competitive candidate for in-situ hydrogen supply; however, the techniques of methanol-to -hydrogen production are suffered from high reforming temperatures and catalyst deactivation. In this work, the chemical looping oxidative reforming of methanol is conducted using a Pd-Cu-based catalytic oxygen carrier (PdO-CuO-CuMn2O4). Synergistic enhancement of lattice oxygen induction and Pd-Cu alloy activation is confirmed, thereby achieving efficient methanol reforming at a temperature as low as 200 degrees C. Under such low temperatures, the hydrogen production rate can reach an average of 11.2 times higher than that of CuO/ZnO/ Al2O3. Moreover, the catalytic oxygen carrier remains relatively satisfying redox durability after 30th cycle. SEM and AFM measurements reveal the high degree of roughness at the PdO-CuO-CuMn2O4 surface, in which the methanol activation can be effectively promoted. XRD and XPS measurements verify the formation of Pd-Cu alloy, as proved by the charge transfer from Pd to Cu. During the redox looping, Pd-Cu alloy is formed and re -separated to be PdO and CuO, thus remaining homogenous distribution of the active phase on an atomic scale. Meanwhile, the lattice oxygen also plays a crucial role in methanol activation, synergistically enhancing the low -temperature reforming of methanol. This study provides a new implication for designing functionalized catalytic oxygen carrier materials, which will substantially promote in-situ hydrogen supply for proton exchange mem-brane fuel cells.