Multimetallic Catalysis in Biology and Synthesis

项目摘要 提出这一行政补充请求是为了资助采购一个微型光纤 UV/可见光/近红外光谱仪，附带软件和采样附件。本设备 将大大加快研究的母奖，其目标是推进多金属 通过解决以下方面的开放性科学问题和挑战来催化：（a）仿生模型 由金属酶激发的络合物，和（B）用于有机合成方法的非生物催化剂。 本赠款周期内的大部分研究计划侧重于主题（a），即 将通过拟议采购的Ocean-HDX-XR光谱仪以及随附的 Ocean Insights提供的采样工具。这一工具将补充现有的核心设施， 该公司提供了一个Windows-95时代的紫外/可见光谱仪，没有近红外功能。不仅 Ocean-HDX-XR是否会为这台老化仪器的灾难性故障提供安全保障， 在近红外区域的光谱窗口，但它也将促进在惰性气氛下的测量 通过无线连接将其转移到手套箱中。增加一个倾角探头附件将 还便于原位反应监测和活性中间体的表征。案例研究是 提出了突出这些增加的能力，了解反应途径的潜在好处 一氧化二氮还原酶的CuZ位点，有氧一氧化碳的Mo/Cu活性位点 脱氢酶，和其他金属酶正在研究的父母奖。

PROJECT SUMMARY This administrative supplement request is proposed to fund procurement of a miniature fiber-optic UV/visible/near-IR spectrometer with accompanying software and sampling accessories. This equipment will significantly accelerate research in the parent award, whose goals are to advance multimetallic catalysis by addressing open scientific questions and challenges regarding (a) biomimetic model complexes inspired by metalloenzymes, and (b) abiological catalysts for organic synthesis methodology. A majority of the research plan during the current grant cycle focused on topic (a), which is the one that will be aided by the proposed procurement of an Ocean-HDX-XR spectrometer with accompanying sampling tools from Ocean Insights. This instrument will complement existing core facilities at the research site, which offer a Windows-95 era UV/visible spectrometer with no near-IR capabilities. Not only will the Ocean-HDX-XR provide security against catastrophic failure of this aging instrument and expand the spectral window in the near-IR region, but it will also facilitate measurements under inert atmosphere by being transferable into gloveboxes using Wifi connectivity. The addition of a dip probe accessory will also facilitate in-situ reaction monitoring and characterization of reactive intermediates. Case studies are presented that highlight the potential benefits of these added capabilities to understand reaction pathways of the CuZ site of nitrous oxide reductase, the Mo/Cu active site of aerobic carbon monoxide dehydrogenase, and other metalloenzymes being studied under the parent award.