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Influence of surface melting effects and availability of reagent ions on LDI-MS efficiency after UV laser irradiation of Pd nanostructures

机译:紫外激光辐照钯纳米结构后表面熔化效应和反应离子的可用性对LDI-MS效率的影响

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In this study, the influence of surface morphology, reagent ions and surface restructuring effects on atmospheric pressure laser desorption/ionization (LDI) for small molecules after laser irradiation of palladium self-assembled nanoparticular (Pd-NP) structures has been systematically studied. The dominant role of surface morphology during the LDI process, which was previously shown for silicon-based substrates, has not been investigated for metal-based substrates before. In our experiments, we demonstrated that both the presence of reagent ions and surface reorganization effects - in particular, melting - during laser irradiation was required for LDI activity of the substrate. The synthesized Pd nanostructures with diameters ranging from 60 to 180nm started to melt at similar temperatures, viz. 890-898K. These materials exhibited different LDI efficiencies, however, with Pd-NP materials being the most effective surface in our experiments. Pd nanostructures of diameters >400-800nm started to melt at higher temperatures, >1000K, making such targets more resistant to laser irradiation, with subsequent loss of LDI activity. Our data demonstrated that both melting of the surface structures and the presence of reagent ions were essential for efficient LDI of the investigated low molecular weight compounds. This dependence of LDI on melting points was exploited further to improve the performance of Pd-NP-based sampling targets. For example, adding sodium hypophosphite as reducing agent to Pd electrolyte solutions during synthesis lowered the melting points of the Pd-NP materials and subsequently gave reduced laser fluence requirements for LDI. Copyright (c) 2015 John Wiley & Sons, Ltd.
机译:在这项研究中,系统地研究了表面形态,试剂离子和表面重构效应对钯自组装纳米颗粒(Pd-NP)结构激光照射后小分子大气压激光解吸/电离(LDI)的影响。在LDI过程中,表面形态的主要作用(以前已显示在硅基衬底上)在此之前尚未进行过研究。在我们的实验中,我们证明了底物的LDI活性需要试剂离子的存在和表面重组效应(特别是熔化)在激光照射过程中都是必需的。直径范围为60至180nm的合成Pd纳米结构在相似的温度下开始熔化。 890-898K。这些材料表现出不同的LDI效率,但是,在我们的实验中,Pd-NP材料是最有效的表面。直径> 400-800nm的Pd纳米结构在> 1000K的更高温度下开始熔化,从而使此类靶标更耐激光辐照,并随后丧失LDI活性。我们的数据表明,表面结构的熔化和试剂离子的存在对于所研究的低分子量化合物的有效LDI至关重要。 LDI对熔点的这种依赖性被进一步利用,以改善基于Pd-NP的采样目标的性能。例如,在合成过程中将次磷酸钠作为还原剂添加到Pd电解质溶液中,降低了Pd-NP材料的熔点,随后降低了LDI的激光注量要求。版权所有(c)2015 John Wiley&Sons,Ltd.

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