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由微等离子体产生的活性物种和短脉冲激光辐照激发的自组织亚微米表面结构

Self-Organizing Sub-μm Surface Structures Stimulated by Microplasma Generated Reactive Species and Short-Pulsed Laser Irradiation.

作者信息

Chur Sascha, Kulik Lennart, Schulz-von der Gathen Volker, Böke Marc, Golda Judith

机构信息

Plasma Interface Physics, Ruhr-University Bochum, 44801 Bochum,Germany.

出版信息

ACS Omega. 2024 Jun 27;9(27):29234-29243. doi: 10.1021/acsomega.3c10033. eCollection 2024 Jul 9.

Abstract

Catalysts are critical components for chemical reactions in industrial applications. They are able to optimize selectivity, efficiency, and reaction rates, thus enabling more environmentally friendly processes. This work presents a novel approach to catalyst functionalization for the CO reduction reaction by combining the reactive species of an atmospheric pressure plasma jet with the electric fields and energy input of a laser. This leads to both a nanoscale structuring as well as a controllable chemical composition of the surface, which are important parameters for optimizing catalyst performance. The treatment is conducted on thin copper layers deposited by high power pulsed magnetron sputtering on silicon wafers. Because atomic oxygen plays a key role in oxidizing copper, two photon absorption fluorescence is used to investigate the atomic oxygen density in the interaction zone of the COST plasma jet and a copper surface. The used atmospheric pressure plasma jet provides an atomic oxygen density at the surface in a distance of 8 mm to the jet nozzle of approximately or a flux of . Pulsed laser-induced dewetting is used to form nanoparticles from the deposited copper layer to enhance catalytic performance. Varying the layer thickness allows control of the size of the particles. A gas flow directed on the sample during the combined treatment disturbs the particle formation. This can be prevented by increasing the laser energy to compensate for the cooling effect of the gas flow. Investigating the surface using X-ray photoemission spectroscopy reveals that the untreated copper layer surface consists mostly of metallic copper and Cu(I) oxide. Irradiating the sample only with the laser did not change the composition. The combination of plasma and laser treatment is able to produce Cu(II) species such as CuO, whose concentration increases with treatment time. The presented process allows the tuning of the ratio of CO/CuO, which is an interesting parameter for further studies on copper catalyst performance.

摘要

催化剂是工业应用中化学反应的关键组成部分。它们能够优化选择性、效率和反应速率,从而实现更环保的工艺。这项工作提出了一种通过将大气压等离子体射流的活性物种与激光的电场和能量输入相结合,对用于CO还原反应的催化剂进行功能化的新方法。这导致了表面的纳米级结构以及可控的化学成分,这些都是优化催化剂性能的重要参数。该处理是在通过高功率脉冲磁控溅射沉积在硅片上的薄铜层上进行的。由于原子氧在氧化铜中起着关键作用,因此使用双光子吸收荧光来研究COST等离子体射流与铜表面相互作用区域中的原子氧密度。所使用的大气压等离子体射流在距喷嘴8 mm处的表面提供的原子氧密度约为 或通量为 。脉冲激光诱导去湿用于从沉积的铜层形成纳米颗粒以提高催化性能。改变层厚度可以控制颗粒的尺寸。在联合处理期间指向样品的气流会干扰颗粒形成。这可以通过增加激光能量来补偿气流的冷却效果来防止。使用X射线光电子能谱对表面进行研究表明,未处理的铜层表面主要由金属铜和Cu(I)氧化物组成。仅用激光照射样品不会改变其成分。等离子体和激光处理的组合能够产生诸如CuO之类的Cu(II)物种,其浓度随处理时间增加。所提出的工艺允许调整CO/CuO的比例,这是进一步研究铜催化剂性能的一个有趣参数。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/05a8/11238218/aecf2934241c/ao3c10033_0001.jpg

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