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通过在不同溶剂中进行脉冲激光烧蚀来制备具有不同形貌的铜纳米粒子及其对还原有毒硝 基芳香族化合物的催化活性。

Production of copper nanoparticles exhibiting various morphologies via pulsed laser ablation in different solvents and their catalytic activity for reduction of toxic nitroaromatic compounds.

机构信息

Department of Chemistry (BK21 FOUR) and Research Institute of Natural Science, Gyeongsang National University, Jinju 52828, Republic of Korea.

Center for Supercomputing Applications, Korea Institute of Science and Technology Information, 245 Daehak-ro, Daejeon 34141, Republic of Korea.

出版信息

J Hazard Mater. 2021 May 5;409:124412. doi: 10.1016/j.jhazmat.2020.124412. Epub 2020 Oct 28.

Abstract

Comparative experiments were conducted to determine the effects of various solvents (i.e., deionized water, methanol, ethanol, 1-propanol, butanol, ethylene glycol, hexane, and acetonitrile) on the final compositions, morphologies, and catalytic activities of copper-based nanoparticles (NPs). The NPs were effectively synthesized by pulsed laser ablation (PLA) using a copper plate as the target. The obtained copper NPs were characterized utilizing various analytical techniques. It was established that the developed methodology allows for the production of NPs with different morphologies and compositions in a safe and simple manner. When laser ablation of a solid copper plate was performed in acetonitrile, the formation of copper(I) cyanide cubes was observed. On the other hand, in deionized water and methanol, spherical and rod-like particles of copper(I) and copper(II) oxide were detected, respectively. The catalytic activity of the prepared copper NPs in the reduction of aromatic nitro compounds, such as 4-nitrophenol and nitrobenzene, was also evaluated. A high k value was determined for the reduction over the copper(II) oxide NPs produced in methanol. Moreover, particles with graphitic carbon (GC) layers exhibited superior catalytic performance in the reduction of a hydrophobic substance, i.e., nitrobenzene, over the reduction of 4-nitrophenol. The enhanced catalytic activity of this catalyst may be due its unique surface morphology and the synergistic effects between the copper nanostructure and the GC layer. Lastly, a detailed reduction pathway mechanism for the catalytic reduction of 4-nitrophenol and nitrobenzene has been proposed.

摘要

进行了对比实验,以确定各种溶剂(即去离子水、甲醇、乙醇、1-丙醇、正丁醇、乙二醇、己烷和乙腈)对铜基纳米粒子(NPs)的最终组成、形态和催化活性的影响。采用脉冲激光烧蚀(PLA)技术,以铜片为靶材,有效地合成了铜 NPs。利用各种分析技术对获得的铜 NPs 进行了表征。结果表明,所开发的方法允许以安全且简单的方式生产具有不同形态和组成的 NPs。当在乙腈中进行固态铜板的激光烧蚀时,观察到形成了铜(I)氰化物立方体。另一方面,在去离子水和甲醇中,分别检测到铜(I)和铜(II)氧化物的球形和棒状颗粒。还评估了所制备的铜 NPs 在还原芳香族硝基化合物(如 4-硝基苯酚和硝基苯)中的催化活性。在甲醇中生成的铜(II)氧化物 NPs 上进行的还原反应的 k 值较高。此外,具有石墨碳(GC)层的颗粒在还原疏水性物质,即硝基苯方面表现出优于还原 4-硝基苯酚的催化性能。该催化剂的增强的催化活性可能归因于其独特的表面形态和铜纳米结构与 GC 层之间的协同效应。最后,提出了催化还原 4-硝基苯酚和硝基苯的详细还原途径机制。

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