In contemporary catalytic interface exploration, experimental studies often take a backseat to theoretical simulations, hindering the development of pristine catalytic interfaces. This research leverages monolayer dispersion theory to design an efficient CO oxidation catalyst through precise manipulation of non-precious metal NiO[sbnd]CeO2 interfaces. Employing the pioneering XRD extrapolation method, we fabricated monolayer dispersed Ni-O-Ce and Ce-O-Ni interfaces, unlocking insights into their impact on the CO oxidation mechanism. The method accurately quantified monolayer dispersion capacities: 0.526 mmol NiO/(100 m2 CeO2) for NiO/CeO2 and 0.0638 mmol CeO2/(100 m2 NiO) for CeO2/NiO, revealing intricate interactions between active components and supports. Utilizing numerical values derived from monolayer dispersion theory, we constructed CeO2-supported NiO (Ni-O-Ce) and NiO-supported CeO2 (Ce-O-Ni) catalysts in a monolayer dispersed state. The Ni-O-Ce interface, generating abundant oxygen vacancies, significantly enhanced CO adsorption and facilitated surface reactive oxygen species production, leading to a remarkable 14-fold increase in intrinsic CO oxidation activity and a notable 4.2-fold improvement in water resistance. Integrating XRD extrapolation, H2-TPR, O2-TPD, CO-TPD, XPS, Raman, and in situ IR techniques, our study demonstrates the feasibility of crafting efficient catalysts with monolayer dispersed atomic-scale catalytic interfaces to elucidate the mechanisms underlying catalytic interface effects on CO oxidation.

The authors are grateful for financial support from the National Natural Science Foundation of China (22062013, 22262021), the Jiangxi Provincial Natural Science Foundation (20212BAB203030, 20232ACB213002, 20192BAB206035), and the Key Laboratory Foundation of Jiangxi Province for Environment and Energy Catalysis (20181BCD40004).

Peer reviewed