腈官能化离子液体 [C3CNC1Im][Tf2N] 在金(111)和铂(111)上的超薄薄膜:吸附、生长和热行为。

IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Langmuir Pub Date : 2024-12-31 Epub Date: 2024-12-16 DOI:10.1021/acs.langmuir.4c04022
Timo Talwar, Jade Barreto, Cynthia Carolina Fernández, Hans-Peter Steinrück, Florian Maier
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引用次数: 0

摘要

研究了硝基功能化离子液体[C3CNC1Im][Tf2N]在150 ~ 600 K范围内对Au(111)和Pt(111)的吸附和热行为。采用物理气相沉积法(PVD)在150 K下制备了超薄膜,并用角分辨x射线光电子能谱(ARXPS)对薄膜进行了表征。在150k时,IL以相似的方向完整地吸附在两个表面上:在第一层,即所谓的湿润层中,阳离子平躺在表面,阴离子以顺式构型结合,SO2基团朝向表面,CF3基团远离表面。在Au(111)上,随后在150 K下多层沉积的IL显示出2D生长直到~ 0.75 ML,并在更高覆盖率下过渡到中等3D。程控温度XPS表明,在220 ~ 290 K之间,湿润层顶部的多层膜的表面形态发生了更明显的3D岛状变化。从350到440 K,多层膜发生解吸,从375-400 K开始分解IL。在更活泼的铂(111)表面,分解在280k以上就开始了。值得注意的是,该温度比相关的非功能化咪唑基il,即[C2C1Im][OTf], [C1C1Im][Tf2N]和[C8C1Im][Tf2N]在Pt(111)上的分解起始温度高~ 80k。这种差异归因于腈的功能。我们的研究结果表明,功能化ILs显着改变了它们的热性能,这与SCILL(具有离子液体层的固体催化剂)系统高度相关。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Ultrathin Films of a Nitrile-Functionalized Ionic Liquid [C3CNC1Im][Tf2N] on Au(111) and Pt(111): Adsorption, Growth, and Thermal Behavior.

We studied the adsorption and thermal behavior of the nitrile-functionalized ionic liquid (IL) [C3CNC1Im][Tf2N] on Au(111) and Pt(111) between 150 and 600 K. Ultrathin films were prepared at 150 K by physical vapor deposition (PVD) and were characterized by angle resolved X-ray photoelectron spectroscopy (ARXPS). At 150 K, the IL adsorbs intact with a similar orientation on both surfaces: In the first layer, the so-called wetting layer, the cation lies flat on the surface and the anion is bound in cis-configuration with the SO2 groups toward the surface and the CF3 groups away from the surface. On Au(111), subsequent deposition of IL in the multilayer regime at 150 K shows 2D growth up until ∼0.75 ML and a transition to moderate 3D at higher coverages. Temperature-programmed XPS indicates a change in surface morphology toward more pronounced 3D islands for the multilayers on top of the wetting layer between 220 and 290 K. From 350 to 440 K, desorption of multilayers occurs, with IL decomposition starting at 375-400 K. On the more reactive Pt(111) surface, decomposition starts already above 280 K. Notably, this temperature is ∼80 K higher than the onset for decomposition of related nonfunctionalized imidazolium-based ILs, that is, [C2C1Im][OTf], [C1C1Im][Tf2N], and [C8C1Im][Tf2N] on Pt(111). This difference is attributed to the nitrile functionality. Our findings demonstrate that functionalizing ILs significantly modifies their thermal properties, which is of high relevance for SCILL (solid catalyst with an ionic liquid layer) systems.

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来源期刊
Langmuir
Langmuir 化学-材料科学:综合
CiteScore
6.50
自引率
10.30%
发文量
1464
审稿时长
2.1 months
期刊介绍: Langmuir is an interdisciplinary journal publishing articles in the following subject categories: Colloids: surfactants and self-assembly, dispersions, emulsions, foams Interfaces: adsorption, reactions, films, forces Biological Interfaces: biocolloids, biomolecular and biomimetic materials Materials: nano- and mesostructured materials, polymers, gels, liquid crystals Electrochemistry: interfacial charge transfer, charge transport, electrocatalysis, electrokinetic phenomena, bioelectrochemistry Devices and Applications: sensors, fluidics, patterning, catalysis, photonic crystals However, when high-impact, original work is submitted that does not fit within the above categories, decisions to accept or decline such papers will be based on one criteria: What Would Irving Do? Langmuir ranks #2 in citations out of 136 journals in the category of Physical Chemistry with 113,157 total citations. The journal received an Impact Factor of 4.384*. This journal is also indexed in the categories of Materials Science (ranked #1) and Multidisciplinary Chemistry (ranked #5).
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