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Updated: Jun 17, 2026

Multiscale Sampling of a Heterogeneous Water/Metal Catalyst Interface using Density Functional Theory and Force-Field Molecular Dynamics
Published on: April 12, 2019
Interface engineering constructs Co-OV-Ce/La interfacial sites with dual "capture-clear" functionality to enhance
Haixiao Sun1, Dongdong Chen1, Wanhong Liu1
1State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum, Beijing 102249, China.
None:
The rational design of interfacial sites is crucial for developing high-performance, water-resistant carbon monoxide (CO) oxidation catalysts. Herein, Co-OV-Ce/La interfacial sites were constructed in cobalt oxide (Co3O4) by co-doping with Ce/La, yielding the La2O3-CeO2@Co3O4 catalyst with outstanding water resistance. At 150 °C under a 20 vol% water (H2O) flow, the catalyst achieved 92% CO conversion, outperforming most previously reported non-precious metal catalysts. The introduction of Ce and La induced lattice distortion, generated oxygen vacancies (OV), activated oxygen species, and enhanced oxidation activity. Especially, OV content in La2O3-CeO2@Co3O4 was increased 1.89-fold compared to pure Co3O4, which promoted the formation of Co-OV-Ce/La interfacial sites. Density functional theory (DFT) indicated that Ce sites at the interface preferentially adsorbed H2O, thereby isolating H2O from Co active sites. Simultaneously, these sites effectively activated surface lattice oxygen by weakening the Co3+-O bond, thereby promoted oxygen migration rates. Combined with in situ diffuse-reflectance Fourier transform infrared spectroscopy (in situ DRIFTS) results, it was found that this interface could effectively promote surface hydroxyl removal and dynamic self-regeneration of interfacial sites in an O2 atmosphere, reducing the accumulation of toxins such as carbonates. Moreover, the La2O3-CeO2@Co3O4 catalyst exhibited excellent thermal stability. This work underscored the critical importance of multi-component interfacial structures in governing catalytic durability and offered a feasible strategy for designing high-performance industrial catalysts under humid conditions.
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