MRI: Track 1 Acquisition of Instrumentation for Marine Metal-Organic and Metalloproteomic Analyses

在环境科学中，自然分子的有机和无机成分通常被分开考虑。然而，近几十年来人们已经清楚，有机-无机界面在生物系统中至关重要：从无机的角度来看，由于金属离子提供的独特化学性质，金属在所有生命形式中都有重要用途。例如，铁和锰在光合作用中是必不可少的，铜、铁和钼是多个关键氮循环反应中的辅助因子，钴、锌甚至镉对碳吸收和细胞内转化至关重要。从有机的角度来看，这些金属通常被各种各样的有机分子所束缚。该项目将支持购买一个现代质谱仪系统，该系统有助于询问有机和无机化学复杂性。该仪器将有助于通过分析大型协调采样工作，如GEOTRACES（包括即将到来的南极GP 17考察），AtriotEco和其他合作项目，测量海洋大区域的金属配体和微生物蛋白质，来了解海洋生物地球化学循环。拟议的仪器还将通过各种合作研究，包括正在进行的与HBCU的合作，以及通过传播新的有机-无机方法，使海洋科学界的研究人员受益。该质谱仪产生的数据将在公共存储库中共享，并纳入海洋蛋白质门户网站，这是一个网络资源，使研究和教育活动（包括基于课堂的研究项目）中使用的非专家用户可以访问组学数据。在这个项目中开发的混合工具将使跨学科的无机-有机研究。具体而言，所获得的轨道阱质谱仪器将通过定制的多维色谱系统耦合到无机等离子体质谱仪，从而可以同时表征复杂的有机分子及其金属含量。由此产生的仪器将使金属配体和溶解有机物表征、金属蛋白质组学和元蛋白质组学领域取得进展，并将加强海洋科学中海洋生物无机化学的新的合作研究。 在这些领域获得的知识将通过研究营养胁迫生物标志物、与地球化学相关的（金属）酶、金属循环和生物利用度来提高对地球化学循环控制的理解。该奖项反映了NSF的法定使命，并被认为值得通过使用基金会的智力价值和更广泛的影响审查标准进行评估来支持。

In environmental sciences, the organic and inorganic components of natural molecules have generally been considered separately. Yet it has become clear in recent decades that the organic-inorganic interface is critically important in biological systems: from the inorganic perspective, there are essential uses of metals in all life forms due to the unique chemical properties metal ions provide. For example, iron and manganese are essential in photosynthesis, copper, iron, and molybdenum are co-factors in multiple key nitrogen cycle reactions, and cobalt, zinc, and even cadmium are critical to carbon uptake and intracellular transformations. And from the organic perspective these metals are typically bound by a wide variety of organic molecules. This project will support the acquisition of a modern mass spectrometer system that contribute to a system capable of interrogating both the organic and inorganic chemical complexities. The instrumentation will contribute to understanding of ocean biogeochemical cycling through the analysis of large, coordinated sampling efforts such as GEOTRACES (including in the upcoming Antarctic GP17 expedition), AtlantEco, and other collaborative projects, measuring metal-ligands and microbial proteins across large regions of the oceans. The proposed instrumentation will also benefit researchers within the ocean science community through a variety of collaborative studies including an ongoing collaboration with a HBCU, as well as through the dissemination of novel organic-inorganic methods. Data produced by this mass spectrometer will be shared on public repositories and incorporated into the Ocean Protein Portal, a web resource that makes ‘omic data accessible to non-expert users used in both research and education activities including class-based research projects. The hybrid instrument developed in this project will enable interdisciplinary inorganic-organic studies. Specifically, the acquired orbitrap mass spectrometry instrumentation will be coupled to an inorganic plasma mass spectrometer via a custom multidimensional chromatographic system allowing simultaneous characterization of complex organic molecules and their metal contents. The resulting instrumentation will enable advances in areas of metal-ligand and dissolved organic matter characterization, metalloproteomics, and metaproteomics and will enhance new collaborative research studies on marine bioinorganic chemistry in the ocean sciences. Knowledge gained in these areas will improve the understanding of controls on Earth’s biogeochemical cycles through the study of nutrient stress biomarkers, biogeochemically relevant (metallo)enzymes, and metal cycling and bioavailability.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.