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

在环境科学中，天然分子的有机成分和无机成分通常被分开考虑。然而，近几十年来已经清楚的是，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必要的用途。例如，铁和锰是光合作用所必需的，铜、铁和钼是多个关键氮循环反应的辅助因素，钴、锌甚至镉是碳吸收和细胞内转化的关键。从有机的角度来看，这些金属通常被各种各样的有机分子结合在一起。该项目将支持购置一个现代质谱仪系统，该系统有助于建立一个能够同时研究有机和无机化学复杂性的系统。该仪器将通过分析大型、协调的采样工作，如GEOTRACES(包括即将进行的南极GP17探险)、AtlantEco和其他合作项目，测量海洋大片区域的金属配体和微生物蛋白质，从而有助于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，包括与HBCU的持续合作，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储存库中共享，并纳入海洋蛋白门户网站，这是一个网络资源，使非专家用户能够访问在研究和教育活动中使用的组学数据，包括基于班级的研究项目。在该项目中开发的混合仪器将使无机-有机跨学科研究成为可能。具体地说，收购的Orbitrap质谱仪将通过定制的多维色谱系统与无机等离子质谱仪耦合，从而同时表征复杂的有机分子及其金属含量。由此产生的仪器将促进金属配体和溶解有机物表征、金属蛋白质组学和偏蛋白质组学领域的进展，并将加强海洋科学中关于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记物、生物地球化学相关(金属)酶以及金属循环和生物有效性来提高对地球生物地球化学循环控制的理解。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

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.