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电置换法制备的金-钯纳米结构:其对元素汞吸附能力优于金的增强作用研究

Galvanically replaced Au-Pd nanostructures: study of their enhanced elemental mercury sorption capacity over gold.

作者信息

Lay B, Sabri Y M, Ippolito S J, Bhargava S K

机构信息

Centre for Advanced Materials and Industrial Chemistry (CAMIC), School of Applied Sciences, RMIT University, Melbourne, 3001, Australia.

出版信息

Phys Chem Chem Phys. 2014 Sep 28;16(36):19522-9. doi: 10.1039/c4cp02233e.

Abstract

In this study, the efficiency of bimetallic (Au-Pd) nanostructures over Au and Pd substrates for elemental mercury (Hg(0)) vapor sensing and capturing was investigated. The quartz crystal microbalance (QCM) technique was utilized to determine the sorption kinetics and quantity of Hg(0) captured by the developed Au-Pd surfaces. The Au-Pd nanostructures were synthesized directly on the QCM's Pd electrodes using galvanic replacement (GR) reactions for periods of 0.5 to 48 hours, which enabled the ratio of Au to Pd on the surface to be controlled. It was observed that the mercury affinity of the surface does not increase with increased Au loading, rather the Au : Pd ratio obtained after a GR reaction time of 1 hour was found to have the highest affinity towards Hg(0) vapor under the GR reaction conditions used in this study. Any further increase in Au : Pd ratio at the surface resulted in reduced affinity for Hg(0) with the Au-rich Au-Pd nanostructures behaving similar to an Au-control substrate. However, short reaction periods (i.e. 1 h) produced small Au nanoparticles increasing the surface to volume ratio for better sensitivity and response times. Remarkably, the QCM data showed that GR based Au-Pd nanostructures removed 2.5 μg cm(-2) of Hg(0) from a gas stream containing 9.1 mg m(-3) of Hg(0) vapor within the first 3 minutes of exposure. The control surfaces (Pd and Au based thin-films) on the other hand took a total of 106 and 159 minutes, respectively to reach the same Hg(0) sorption capacity from the same gas stream.

摘要

在本研究中,研究了双金属(金 - 钯)纳米结构在金和钯基底上对元素汞(Hg(0))蒸汽的传感和捕获效率。利用石英晶体微天平(QCM)技术来确定所开发的金 - 钯表面捕获Hg(0)的吸附动力学和量。通过电置换(GR)反应在QCM的钯电极上直接合成金 - 钯纳米结构,反应时间为0.5至48小时,这使得表面上金与钯的比例能够得到控制。观察到表面对汞的亲和力并不随金负载量的增加而增加,相反,发现在本研究使用的GR反应条件下,GR反应1小时后获得的金∶钯比例对Hg(0)蒸汽具有最高的亲和力。表面上金∶钯比例的任何进一步增加都会导致对Hg(0)的亲和力降低,富金的金 - 钯纳米结构的行为类似于金对照基底。然而,短反应时间(即1小时)会产生小的金纳米颗粒,增加了表面积与体积比,从而具有更好的灵敏度和响应时间。值得注意的是,QCM数据表明,基于GR的金 - 钯纳米结构在暴露的前3分钟内从含有9.1 mg m(-3) Hg(0)蒸汽的气流中去除了2.5 μg cm(-2)的Hg(0)。另一方面,对照表面(基于钯和金的薄膜)分别总共需要106分钟和159分钟才能从相同的气流中达到相同的Hg(0)吸附容量。

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