Collaborative Research: Molecular Level Characterization of Organic Matter in Ice Cores using high-resolution FTICR mass spectrometry

合作研究：使用高分辨率 FTICR 质谱法对冰芯中有机物进行分子水平表征

• 批准号: 0739691
• 负责人: Amanda Grannas
• 金额: $ 17.9万
• 依托单位: Villanova University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2008
• 资助国家: 美国
• 起止时间: 2008-09-01 至 2013-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0739691&HistoricalAwards=false
• 关键词: Collaborative; Research; Molecular; Level; Characterization

Grannas/0739691This award supports a project to fully develop the analytical protocols needed to exploit a relatively new technique for the analysis of soluble organic matter in ice core samples. The technique couples Electrospray ionization to high resolution Fourier transform ion cyclotron resonance mass spectrometry (ESI-FTICR-MS). Sample volume will be reduced and pre-concentration steps will be eliminated. Following method optimization a suite of ice core samples will be studied from several Antarctic and Greenland locations to address several hypothesis driven research questions. Preliminary results show that a vast record of relatively high molecular weight organic material exists in ice core samples and intriguing results from a few samples warrant further investigation. Several important questions related to developing a better understanding of the nature and paleo record of organic matter in ice cores will be addressed. These include developing a better understanding of the origin of nitrogen and sulfur isotopes in pre-industrial vs. modern samples, developing the methods to apply molecular biomarker techniques, routinely used by organic geochemists for sediment analyses, to the analysis of organic matter in ice cores, tracking the level of oxidation of homologous series of compounds and using them as a proxy for atmospheric oxidant levels in the past and determining whether or not high resolution FTICR mass spectral analysis can provide the ice core community with a robust method to analyze organic materials at the molecular level. The intellectual merit of this work is that this analytical method will provide a new understanding of the nature of organic matter in ice, possibly leading to the discovery of multitudes of molecular species indicative of global change processes whose abundances can be compared with other change proxies. The proposed studies are of an exploratory nature and potentially transformative for the field of ice core research and cryobiology. The broader impacts of these studies are that they should provide compelling evidence regarding organic matter sources, atmospheric processing and anthropogenic inputs to polar ice and how these have varied over time. The collaborative work proposed here will partner atmospheric chemistry/polar ice chemistry expertise with organic geochemistry expertise, resulting in significant contributions to both fields of study and significant advances in ice core analysis. Training of both graduate and undergraduate students will be a key component of the project and students will be involved in collaborative research using advanced analytical instrumentation, presentation of research results at national meetings, and will participate in manuscript preparation.

Grannas/0739691该奖项支持一个项目，以充分开发所需的分析协议，以利用一种相对较新的技术来分析冰芯样品中的可溶性有机物。 该技术将电喷雾电离与高分辨率傅里叶变换离子回旋共振质谱（ESI-FTICR-MS）相结合。 将减少样品体积，并取消预浓缩步骤。在方法优化之后，将对来自南极和格陵兰几个地点的一套冰芯样品进行研究，以解决几个假设驱动的研究问题。 初步结果表明，冰芯样品中存在大量相对高分子量的有机物质，少数样品的有趣结果值得进一步研究。与发展更好地了解冰芯中有机物的性质和古记录有关的几个重要问题将得到解决。其中包括更好地了解工业化前与现代样品中氮和硫同位素的来源，开发将有机地球化学家经常用于沉积物分析的分子生物标志物技术应用于冰芯中有机物分析的方法，追踪同系化合物的氧化水平，并将其用作过去大气氧化剂水平的代表，并确定高分辨率FTICR质谱分析是否可以为冰芯群落提供一种在分子水平上分析有机物质的可靠方法。 这项工作的智力价值是，这种分析方法将使人们对冰中有机物的性质有新的认识，可能导致发现大量的分子种类，这些分子种类表明全球变化过程，其丰度可与其他变化代用指标进行比较。 拟议的研究是一个探索性的性质和潜在的变革领域的冰芯研究和低温生物学。 这些研究的更广泛影响是，它们应该提供令人信服的证据，说明有机物质来源、大气处理和人为输入极地冰以及这些如何随时间变化。这里提议的合作工作将使大气化学/极地冰化学专门知识与有机地球化学专门知识结成伙伴关系，从而对这两个研究领域作出重大贡献，并在冰芯分析方面取得重大进展。对研究生和本科生的培训将是该项目的一个关键组成部分，学生将参与使用先进分析仪器的合作研究，在国家会议上介绍研究成果，并将参与手稿准备。