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非均相铑基固溶体合金纳米颗粒的催化活性增强

Enhanced catalytic activity of inhomogeneous Rh-based solid-solution alloy nanoparticles.

作者信息

Sarker Md Samiul Islam, Nakamura Takahiro, Kameoka Satoshi, Hayasaka Yuichiro, Yin Shu, Sato Shunichi

机构信息

Department of Physics, University of Rajshahi Rajshahi 6205 Bangladesh

Institute of Multidisciplinary Research for Advanced Materials (IMRAM), Tohoku University Katahira 2-1-1, Aoba-ku Sendai 980-8577 Japan

出版信息

RSC Adv. 2019 Nov 27;9(66):38882-38890. doi: 10.1039/c9ra06167c. eCollection 2019 Nov 25.

Abstract

Catalytic Rh-based alloy nanoparticles (NPs) with inhomogeneous solid-solution structures were prepared from homogeneous solid-solution alloy NPs. Compared with homogeneous alloy NPs, these inhomogeneous alloy NPs exhibited enhanced catalytic activity and superior catalytic durability. Homogeneous solid-solution alloy NPs consisting of Rh and other immiscible noble metals were synthesized by laser-induced nucleation method in metallic ion solutions. STEM elemental mapping and EDS composition analysis of the particles clearly demonstrated that all the constituents were uniformly dispersed within the NPs. Moreover, the compositions of the alloys were nearly identical to the initial feeding ratios of metallic ions in the mixed solutions, strongly indicating the formation of equimolar solid-solution alloy NPs over the entire composition range. Although the catalytic stability of these Rh-based homogeneous alloy NPs during CO oxidation was improved, their catalytic activity was comparable to that of pure metal catalysts, owing to the uniform local structure at the atomic level. However, the catalytic activity of the alloy NPs was enhanced by heat treatment, which introduced inhomogeneity in the atomic distribution within the NPs. The enhanced activity was due to dissimilar interfaces in the inhomogeneous solid-solution alloy NPs.

摘要

由均匀固溶体合金纳米颗粒制备出具有非均匀固溶体结构的催化铑基合金纳米颗粒。与均匀合金纳米颗粒相比,这些非均匀合金纳米颗粒表现出更高的催化活性和卓越的催化耐久性。通过激光诱导成核法在金属离子溶液中合成了由铑和其他不混溶贵金属组成的均匀固溶体合金纳米颗粒。对颗粒进行的扫描透射电子显微镜(STEM)元素映射和能谱(EDS)成分分析清楚地表明,所有成分都均匀地分散在纳米颗粒内。此外,合金的成分几乎与混合溶液中金属离子的初始进料比相同,这有力地表明在整个成分范围内形成了等摩尔固溶体合金纳米颗粒。尽管这些铑基均匀合金纳米颗粒在一氧化碳氧化过程中的催化稳定性有所提高,但由于原子水平上的均匀局部结构,它们的催化活性与纯金属催化剂相当。然而,通过热处理提高了合金纳米颗粒的催化活性,热处理在纳米颗粒内的原子分布中引入了不均匀性。活性增强是由于非均匀固溶体合金纳米颗粒中存在不同的界面。

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