Guo Song, Zhang Guomei, Han Zhong-Kang, Zhang Shaoyang, Sarker Debalaya, Xu Wen Wu, Pan Xiaoli, Li Gao, Baiker Alfons
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, China.
ACS Appl Mater Interfaces. 2021 Jan 13;13(1):622-630. doi: 10.1021/acsami.0c18451. Epub 2020 Dec 23.
We developed a robust ternary PdO-CeO-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 at the nearly full conversion of NO and CO at 250 °C, high stability in the presence of HO, and a remarkable SO tolerance. To unravel the origin of the excellent catalytic performance, the structural and chemical properties of the PdO-CeO-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 and Pd), while NO decomposes on the ceria surface. Lattice oxygen vacancies at the interfacial perimeter of PdO-CeO and PdO-OMS-2, and the diffusion of oxygen and oxygen vacancies are proposed to play a critical role in this multicenter reaction system.
我们通过一种基于组合具有协同相互作用的组分的策略,开发了一种在CO选择性还原NO反应中具有优异催化性能的稳健三元PdO-CeO-OMS-2催化剂,从而有效消除这些有毒气体。该催化剂在250℃下NO和CO几乎完全转化时对N具有100%的选择性,在HO存在下具有高稳定性,并且具有显著的SO耐受性。为了揭示优异催化性能的来源,采用一系列相关表征方法和特定催化测试,对PdO-CeO-OMS-2纳米复合材料在催化剂的制备态和使用态下的结构和化学性质进行了分析。基于密度泛函理论计算的实验和理论结果表明,CO和NO遵循不同的反应途径,CO优先在Pd位点(Pd和Pd)上吸附和氧化,而NO在二氧化铈表面分解。PdO-CeO和PdO-OMS-2界面周边的晶格氧空位以及氧和氧空位的扩散被认为在这个多中心反应体系中起关键作用。