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A QCM-based 'on-off' mechanistic study of gas adsorption by plasmid DNA and DNA-[Bmim][PF6] construct

机译:基于QCM的“QCM的”ON-OFF“质粒吸附质粒DNA和DNA-[BMIM] [PF6]构建体

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摘要

The study of the adsorption behavior of disease markers such as ammonia (NH3) and acetaldehyde (CH3CHO) with biomaterials is important, as it will improve our understanding of their interaction behavior and enable the development of self-diagnosis technologies, among others. In this study, three types of DNA-based biomaterials were synthesized (pGFP plasmid DNA isolated from E. coli DH5 alpha, a DNA-ionic liquid construct (DNA-IL) and DNA-ionic liquid-gold chloride (DNA-IL-Au)) and their adsorption capacities for NH3 and CH3CHO were tested by utilizing a gravimetric transducer, namely, a quartz crystal microbalance (QCM). Pristine DNA itself displayed high sensitivity towards both gases, with a pristine DNA-based QCM displaying magnitudes of response of similar to 3.74 and 2.62 ng cm(-2) mu g(-1) following 10 minutes of exposure to 600 ppm NH3 and CH3CHO, respectively. Interestingly, no response was observed when these gases were exposed to the DNA-IL complex, which comprised DNA modified with the hydrophobic IL [Bmim][PF6]. However, when the DNA-IL complex was further treated with HAuCl4, the biomaterial (DNA-IL-Au) regained its adsorption capacity, exhibiting magnitudes of adsorption/response up to 140% and 36% higher than its DNA counterpart toward NH3 and CH3CHO, respectively. It was also observed that the utilization of DNA-IL-Au significantly reduced the sensitivity of the QCM device to humidity content, which indicates that the developed biomaterial can be readily employed to detect NH3 and CH3CHO in humid environments. Further study showed that the magnitudes of the QCM response of the DNA and DNA-IL-Au materials toward the different concentrations of NH3 and CH3CHO that were tested follow the loading ratio correlation (LRC), which thus indicates that the developed materials can potentially be utilized as sensitive layers for the detection of biomarker gases that are produced in the body as a result of biomedical disorders. In addition, a plausible sorption mechanism has also been proposed on the basis of the interaction of DNA with the ionic liquid and HAuCl4 (experimentally proved by XPS and FTIR), which strongly indicates the role of the phosphates and nucleobases of DNA for the electrostatic binding of NH3 and CH3CHO, respectively.
机译:疾病标志物如氨(NH3)和乙醛(CH3CHO)与生物材料吸附行为的研究是很重要的,因为这将提高我们它们的相互作用行为的理解和支持的自诊断技术的发展,等等。在这项研究中,三种类型的基于DNA的生物材料的合成(pGFP质粒DNA从大肠杆菌DH5α,一个DNA的离子液体构建体(DNA-IL)和DNA的离子型液体,氯化金(DNA-IL-分离的Au ))和NH 3和CH3CHO它们的吸附能力得到通过利用重力传感器测试,即,石英晶体微量天平(QCM)。原始DNA本身显示高灵敏度朝向两种气体,与显示的类似响应的幅度质朴的基于DNA的QCM到3.74和2.62纳克厘米(-2)亩克(-1)以下暴露10分钟的至600ppm NH 3和CH3CHO , 分别。有趣的是,当这些气体暴露于DNA-IL复合物,其由DNA修饰与疏水性IL [BMIM] [PF 6]未观察到响应。然而,当DNA-IL复合物进一步用氯金酸处理,生物材料(DNA-IL-Au)的恢复了它的吸附能力,显示出吸附/响应的幅度高达140%和36%高于其DNA对应物朝向NH3和CH3CHO , 分别。还观察到,即DNA-IL-Au构成的利用率显著降低QCM装置湿度含量,这表明生物材料发达可容易地用于检测NH 3和CH3CHO在潮湿环境中的灵敏度。进一步的研究表明,朝向进行了测试遵循负载率相关(LRC),其因此表示开发材料可以潜在地是不同浓度的NH 3和CH 3 CHO的DNA和DNA-IL-金材料的QCM响应的幅度用作对于在体内产生的生物医学病症的结果的生物标记物的气体的检测敏感层。此外,一个合理的吸附机理还提出了DNA的与离子液体和氯金酸(由XPS和FTIR实验证明),其强烈表明DNA的磷酸盐和核碱基的用于静电结合的作用的相互作用的基础上的分别NH3和CH3CHO,。

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  • 来源
    《RSC Advances》 |2016年第84期|共12页
  • 作者单位

    RMIT Univ Sch Sci Ctr Adv Mat &

    Ind Chem Melbourne Vic 3001 Australia;

    RMIT Univ Sch Sci Ctr Adv Mat &

    Ind Chem Melbourne Vic 3001 Australia;

    CSIRO Mfg Flagship Clayton South MDC Private Bag 10 Clayton Vic 3169 Australia;

    RMIT Univ Sch Sci Ctr Adv Mat &

    Ind Chem Melbourne Vic 3001 Australia;

    RMIT Univ Sch Sci Melbourne Vic 3001 Australia;

    RMIT Univ Sch Sci Ctr Adv Mat &

    Ind Chem Melbourne Vic 3001 Australia;

    RMIT Univ Sch Sci Ctr Adv Mat &

    Ind Chem Melbourne Vic 3001 Australia;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 化学;
  • 关键词

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