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通过 Pt/FeO 催化剂中 FeO{113} 晶面依赖性效应促进汽车尾气碳颗粒的催化净化。

Facilitating Catalytic Purification of Auto-Exhaust Carbon Particles via the FeO{113} Facet-dependent Effect in Pt/FeO Catalysts.

机构信息

State Key Laboratory of Heavy Oil Processing, Key Laboratory of Optical Detection Technology for Oil and Gas, China University of Petroleum, Beijing 102249, P. R. China.

Key Laboratory of Beijing on Regional Air Pollution Control, Beijing Key Laboratory for Green Catalysis and Separation, Beijing University of Technology, Beijing 100124, China.

出版信息

Environ Sci Technol. 2021 Dec 7;55(23):16153-16162. doi: 10.1021/acs.est.1c05908. Epub 2021 Nov 19.

Abstract

The purification efficiency of auto-exhaust carbon particles in the catalytic aftertreatment system of vehicle exhaust is strongly dependent on the interface nanostructure between the noble metal component and oxide supports. Herein, we have elaborately synthesized the catalysts (Pt/FeO-R) of Pt nanoparticles decorated on the hexagonal bipyramid α-FeO nanocrystals with co-exposed twelve {113} and six {104} facets. The area ratios () of co-exposed {113} to {104} facets in α-FeO nanocrystals were adjusted by the fluoride ion concentration in the hydrothermal method. The strong Pt-FeO{113} facet interaction boosts the formation of coordination unsaturated ferric sites for enhancing adsorption/activation of O and NO. Pt/FeO-R catalysts exhibited the FeO{113} facet-dependent performance during catalytic purification of soot particles in the presence of HO. Among the catalysts, the Pt/FeO-19 catalyst exhibits the highest catalytic activities ( = 365 °C, TOF = 0.13 h), the lowest apparent activation energy (69 kJ mol), and excellent catalytic stability during soot purification. Combined with the results of characterizations and density functional theory calculations, the catalytic mechanism is proposed: the active sites located at the Pt-FeO{113} interface can boost the key step of NO oxidation to NO. The crystal facet engineering is an effective strategy to obtain efficient catalysts for soot purification in practical applications.

摘要

汽车尾气催化后处理系统中自动排气碳颗粒的净化效率强烈依赖于贵金属组分与氧化物载体之间的界面纳米结构。在此,我们精心合成了 Pt 纳米颗粒负载在具有共暴露的十二 {113} 和六 {104} 面的六方双锥 α-FeO 纳米晶上的催化剂 (Pt/FeO-R)。通过水热法中的氟离子浓度来调整 α-FeO 纳米晶中共同暴露的 {113} 面与 {104} 面的面积比 ()。Pt-FeO{113} 面的强相互作用促进了配位不饱和铁位的形成,从而增强了 O 和 NO 的吸附/活化。Pt/FeO-R 催化剂在存在 HO 的情况下对炭黑颗粒的催化净化过程中表现出 FeO{113} 面依赖性的性能。在这些催化剂中,Pt/FeO-19 催化剂表现出最高的催化活性 ( = 365°C,TOF = 0.13 h)、最低的表观活化能 (69 kJ mol) 和在炭黑净化过程中的优异催化稳定性。结合表征和密度泛函理论计算的结果,提出了催化机理:位于 Pt-FeO{113} 界面的活性位点可以促进 NO 氧化到 NO 的关键步骤。晶面工程是获得实际应用中炭黑净化高效催化剂的有效策略。

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