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原子级铂位点锚定在富空位的CeO纳米片晶粒间界面:一步前驱体燃烧合成法

Atomic Pt Sites Anchored in the Interface between Grains on Vacancy-Enriched CeO Nanosheets: One-Step Precursor Combustion Synthesis.

作者信息

Dong Feng, Liang Xiao, Zhang Zedong, Yin Haibo, Wang Dingsheng, Li Junhua, Li Yadong

机构信息

Department of Chemistry, Tsinghua University, Beijing, 100084, China.

State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing, 100084, China.

出版信息

Adv Mater. 2024 Jun;36(25):e2401055. doi: 10.1002/adma.202401055. Epub 2024 Apr 9.

Abstract

Atomic metal catalysts have unique electronic, structural, and catalytic properties, which are widely used in the field of catalysis. However, designing new simple synthesis methods to fabricate atomic metal catalysts is a challenge in catalytic applications. Herein, a one-step precursor combustion strategy is presented that starts directly from precursors of metal salts, using a spontaneous combustion process convert platinum nitrate to atomic Pt sites. The atomic Pt sites with low valence are anchored in the formed interface between grains on vacancy-enriched CeO nanosheets. The obtained Pt/CeO-2 catalyst exhibits much higher three-way catalytic activities at low temperatures than Pt/CeO-C catalysts prepared using the traditional impregnation method. Density functional theory calculations show that the generated lower valent Pt atoms in the CeO interface promote catalytic activity through reducing the energy barrier, and lead to an overall improvement of three-way catalytic activities. This facile strategy provides new insights into the study of the properties and applications of atomic noble metal catalysts.

摘要

原子金属催化剂具有独特的电子、结构和催化性能,在催化领域得到广泛应用。然而,设计新的简单合成方法来制备原子金属催化剂是催化应用中的一个挑战。在此,提出了一种一步前驱体燃烧策略,该策略直接从金属盐前驱体开始,利用自燃过程将硝酸铂转化为原子级Pt位点。低价的原子级Pt位点锚定在富含空位的CeO纳米片上晶粒间形成的界面处。所制备的Pt/CeO₂催化剂在低温下比采用传统浸渍法制备的Pt/CeO-C催化剂表现出更高的三效催化活性。密度泛函理论计算表明,CeO界面中生成的低价Pt原子通过降低能垒促进催化活性,从而导致三效催化活性的整体提高。这种简便的策略为原子级贵金属催化剂的性能和应用研究提供了新的思路。

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