期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 1, 页码 622-630出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c18451
关键词
NO reduction with CO; PdO-CeO2-OMS-2 nanocomposite catalyst; H2O and SO2 tolerance; synergistic effects in multicomponent system; long-term stability; reaction mechanism
资金
- National Natural Science Foundation of China [21773189, 11974195]
- Liaoning Natural Science Foundation of China [2020-MS-024]
- Liaoning Revitalization Talents Program [XLYC1807121]
The ternary PdO-CeO2-OMS-2 catalyst shows excellent performance in selectively reducing NO and CO, converting them nearly completely to N-2. Analysis of the catalyst's structural and chemical properties reveals the crucial role of lattice oxygen vacancies and oxygen diffusion in this multicenter reaction system.
We developed a robust ternary PdO-CeO2 -OMS-2 catalyst with excellent catalytic performance in the selective reduction of NO with CO using a strategy based on combining components that synergistically interact leading to an effective abatement of these toxic gases. The catalyst affords 100% selectivity to N-2 at the nearly full conversion of NO and CO at 250 degrees C, high stability in the presence of H2O, and a remarkable SO2 tolerance. To unravel the origin of the excellent catalytic performance, the structural and chemical properties of the PdO-CeO2-OMS-2 nanocomposite were analyzed in the as-prepared and used state of the catalyst, employing a series of pertinent characterization methods and specific catalytic tests. The experimental as well as theoretical results, based on density-functional theory calculations suggest that CO and NO follow different reaction pathways, CO is preferentially adsorbed and oxidized at Pd sites (Pd-II and Pd-0), while NO decomposes on the ceria surface. Lattice oxygen vacancies at the interfacial perimeter of PdO-CeO2 and PdO-OMS-2, and the diffusion of oxygen and oxygen vacancies are proposed to play a critical role in this multicenter reaction system.
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