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研究发现将二氧化铈转化成二维团簇可以增强催化活性
作者:小柯机器人 发布时间:2025/4/10 17:27:38

近日,美国太平洋西北国家实验室教授王勇及其研究组发现,将二氧化铈转化成二维团簇可以增强催化活性。这一研究成果发表在2025年4月9日出版的国际学术期刊《自然》上。

在这里,该课题组研究人员发现在750到1000 通过显微镜、x射线光电子能谱(XPS)、x射线吸收光谱(XAS)、红外光谱和密度泛函理论(DFT)计算证实,在蒸汽中CO和NO存在的°C下(还原气氛下的反应处理),导致二氧化铈纳米粒子分散到高密度的2D(大约一个原子层薄)CexOy畴中。这些结构域密集地覆盖在氧化铝表面,表现出显著增强的氧迁移和存储能力,有利于氧气的提取和Ce3+位点和氧空位的形成。因此,这些催化剂——无论是否含有PGMs,如Rh和Pt——在一些重要的催化反应中表现出更高的活性,包括NO和N2O的还原,以及CO和NO的氧化,即使在恶劣的老化条件下也是如此。本研究展示了一种催化剂结构,在典型的烧结条件下具有优异的氧化还原性能,为更有效的金属-二氧化铈催化剂的增强一般催化提供了途径。

据悉,氧化铝负载的氧化铈纳米颗粒广泛应用于各种催化反应,特别是与铂族金属(PGMs)结合使用。

附:英文原文

Title: Transforming ceria into 2D clusters enhances catalytic activity

Author: Khivantsev, Konstantin, Pham, Hien, Engelhard, Mark H., Aleksandrov, Hristiyan A., Kovarik, Libor, Bowden, Mark, Li, Xiaohong Shari, Tian, Jinshu, Koleva, Iskra Z., Song, Inhak, Hu, Wenda, Wei, Xinyi, Sun, Yipeng, Tran, Pascaline, Graham, Trent R., Jiang, Dong, Dean, David P., Breckner, Christian J., Miller, Jeffrey T., Vayssilov, Georgi N., Szanyi, Jnos, Datye, Abhaya, Wang, Yong

Issue&Volume: 2025-04-09

Abstract: Ceria nanoparticles supported on alumina are widely used in various catalytic reactions, particularly in conjunction with platinum group metals (PGMs)1,2,3,4,5,6,7,8,9. Here we found that treating these catalysts at temperatures between 750 and about 1,000°C in the presence of CO and NO in steam (reactive treatment under reducing atmosphere) leads to the dispersion of ceria nanoparticles into high-density 2D (roughly one atomic layer thin) CexOy domains, as confirmed by microscopy, X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy (XAS), infrared spectroscopy and density functional theory (DFT) calculations. These domains, which densely cover the alumina, exhibit substantially enhanced oxygen mobility and storage capacity, facilitating easier extraction of oxygen and the formation of Ce3+ sites and oxygen vacancies. As a result, these catalysts—whether with or without PGMs, such as Rh and Pt—show improved activity for several industrially important catalytic reactions, including NO and N2O reduction, as well as CO and NO oxidation, even after exposure to harsh ageing conditions. This study shows a catalyst architecture with superior redox properties under conditions that typically cause sintering, offering a pathway to more efficient metal–ceria catalysts for enhanced general catalysis.

DOI: 10.1038/s41586-025-08684-x

Source: https://www.nature.com/articles/s41586-025-08684-x

期刊信息
Nature:《自然》,创刊于1869年。隶属于施普林格·自然出版集团,最新IF:69.504
官方网址:http://www.nature.com/