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

机译：增强非均匀RH基固溶合金纳米粒子的催化活性

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摘要

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.
机译：催化Rh基合金纳米颗粒（NPS）由均匀固溶体合金NPS制备非均匀固溶体结构。与均相合金NPS相比，这些不均匀合金NPS表现出增强的催化活性和优异的催化耐久性。通过在金属离子溶液中的激光诱导的成核法合成了由RH和其他不混溶的贵金属组成的均匀固溶合金NPS。茎元素映射和颗粒的编辑组成分析清楚地证明，所有成分均匀地分散在NPS内。此外，合金的组合物几乎与混合溶液中金属离子的初始进料比相同，强烈表示在整个组成范围内形成等摩尔固溶合金NP的形成。尽管在共氧化过程中，这些Rh基均匀合金NP的催化稳定性得到改善，但由于原子水平均匀的局部结构，它们的催化活性与纯金属催化剂的催化活性相当。然而，通过热处理增强了合金NP的催化活性，其在NPS内引入原子分布中的不均匀性。增强的活性是由于非均匀固溶合金NPS中的不同界面。

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