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在负载型 Pd 纳米颗粒还原 NO 过程中的反应活性:揭示金属-载体氧化还原相互作用。

On the reactivity of carbon supported Pd nanoparticles during NO reduction: unraveling a metal-support redox interaction.

机构信息

Instituto de Física, Universidade Federal do Rio Grande do Sul (UFRGS), Porto Alegre, RS, Brazil.

出版信息

Langmuir. 2013 Jun 11;29(23):7125-33. doi: 10.1021/la401460c. Epub 2013 May 31.

DOI:10.1021/la401460c
PMID:23683147
Abstract

Pd nanoparticles (NPs) were successfully obtained by the reduction of PdCl2 with L-ascorbic acid, whose morphology was revealed by HRTEM to be a worm-like system, formed by linked crystallite clusters with an average short-axis diameter of 5.42 nm. In situ UV-vis absorption measurements were used to monitor their formation, while XPS and XRD characterization confirmed the NPs' metallic state. A straightforward way to support the obtained Pd NPs on activated carbon (AC) was used to prepare a catalyst for NO decomposition reaction. The Pd/AC catalysts proved to be highly active in the temperature range of 323 to 673 K, and a redox mechanism is proposed, where the catalyst's active sites are oxidized by NO and reduced by carbon, emitting CO2 and enhancing their capacity to absorb and dissociate NO.

摘要

钯纳米粒子(NPs)通过 L-抗坏血酸还原 PdCl2 成功获得,其形态通过高分辨透射电子显微镜(HRTEM)揭示为一种蠕虫状系统,由连接的微晶簇组成,平均短轴直径为 5.42nm。原位紫外-可见吸收测量用于监测其形成,而 X 射线光电子能谱(XPS)和 X 射线衍射(XRD)表征证实了 NPs 的金属态。一种简单的方法是将获得的 Pd NPs 负载在活性炭(AC)上,以制备用于 NO 分解反应的催化剂。Pd/AC 催化剂在 323 至 673 K 的温度范围内表现出高活性,并提出了一种氧化还原机制,其中催化剂的活性位点被 NO 氧化,被碳还原,释放出 CO2 并增强其吸收和解离 NO 的能力。

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