Multi-user, High-Throughput Facility for Compositional Analysis of Molecules and Materials

确定样品的元素组成在实验化学的所有学科中都是必不可少的。虽然核磁共振(核磁共振)和质谱学(MS)等光谱方法提供了有关连接性的补充信息，但元素分析(EA)的高灵敏度和相独立使其成为i)表征不溶固体、ii)对其他技术(例如核磁共振-无声核、3-D材料)不敏感的样品以及iii)评估整体纯度的金标准。 自2018年启动以来，主要申请者已经建立了一个国际公认的战略分子设计计划，以从主要族元素中获得新的性质(见《化学》中的简介)。交警。新兴研究人员问题，9本独立出版物，特邀书籍章节，2年内组织的2次会议)。该计划的一个关键方面涉及使用几何设计来获得从根本上新型的材料，这些材料在骨骼中包含3D分子笼。由于它们的全杂原子骨架和笼状结构，这些聚合物具有刚性棒系统的导电性和物理性能的可移动电子，使它们成为潜在的有价值的电子和结构材料。由这种聚合物衍生的网络可以作为形状限定的金属磷化物陶瓷的前体。要描述这些迷人但不可溶的固态材料，需要高频地进行C、H、N、S、O分析(绘制组成它们的5/6元素图)。缺乏这些数据，主要申请者无法继续进行，从而失去了有影响力的科学和他作为职业生涯敏感阶段公认的领导者的地位。EA数据对该项目至关重要，并将在发生时立即提供可操作的见解来指导研究。例如，为了获得高相对分子质量的无机聚合物、解释聚合动力学和检测端基，需要对单体批次进行频繁的分析。陶瓷中的有机残留物也必须量化，因为它们的功能特性(例如导电性)会受到此类杂质的影响。 除主要申请人外，另外6个组(Freund、Thompson、Turculet、斯特拉迪奥托、Speed、Doucette)因及时获取这些数据而受到严重阻碍，因为样品要么不适用于解决方法，要么太敏感，无法在外部设施以不可预测的延迟进行分析。这一数据在催化中是至关重要的，在催化中，杂质可以介导副反应，在更广泛的合成化学中，当涉及盐的歧化反应(涉及核磁共振无声的金属卤化物或自由基)时，这些数据是至关重要的。EA数据还提供了蛋白质组学研究中的关键见解，作为对从生物系统中回收蛋白质的分析物的公正评估。 有鉴于此，这项来自4个学科多个职业阶段的7名研究人员的联合申请寻求资金，以建立一个能够高通量进行C、H、N、S、O分析的系统。

Establishing the elemental composition of samples is essential across all disciplines of experimental chemistry. While spectroscopic methods such as nuclear magnetic resonance (NMR) and mass spectrometry (MS) provide complementary information about connectivity, the high-sensitivity and phase-independence of elemental analysis (EA) makes it the gold standard for i) characterizing insoluble solids, ii) for samples that are unresponsive to other techniques (e.g. NMR-silent nuclei, 3-D materials), and iii) for assessing bulk purity. Since starting up in 2018, the principal applicant has established an internationally recognized program of strategic molecular design to elicit new properties from main group elements (see profile in Chem. Commun. Emerging Investigators Issue, 9 independent publications, invited book chapter, 2 conferences organized in 2 years). A key aspect of this program involves using geometric design to access fundamentally new types of materials that contain 3-D molecular cages in the back bone. Due to their all-heteroatom backbone and cage microstructure, these polymers have mobile electrons for conductivity and physical properties of rigid-rod systems, making them potentially valuable electronic and structural materials. Networks derived from such polymers behave as precursors to shape-defined metal phosphide ceramics. Characterizing these fascinating but insoluble solid-state materials requires high-frequency access to C, H, N, S, O analysis (to map 5/6 elements comprising them). Lacking this data, the principal applicant is unable to proceed, thereby forfeiting impactful science and his position as a recognized leader at a sensitive career stage. EA data is critical to this project and will provide immediately actionable insights to guide research in the moment it happens. For example, frequent assays of monomer batches are required to access high molecular weight inorganic polymers, interpret polymerization kinetics, and detect end groups. The organic residue in ceramics must also be quantified as their functional properties (e.g. conductivity) are influenced by such impurities. Besides the principal applicant, 6 additional groups (Freund, Thompson, Turculet, Stradiotto, Speed, Doucette) are critically impeded by timely access to this data as samples are either not amenable to solution methods or too sensitive to be analyzed at external facilities with unpredictable delays. This data is vital in catalysis, where impurities can mediate side-reactions, and in synthetic chemistry more broadly when salt metathesis reactions (involving NMR-silent metal halides or radicals) are involved. EA data also provides key insights in proteomics research as an unbiased evaluation of analyte recovery for proteins from biological systems. In light of the above, this joint application from 7 researchers spanning multiple career stages across 4 disciplines seeks funding for a system capable of high-throughput C, H, N, S, O analysis.