Determining Mechanisms and Energetics of Alkane Activation and Coupling by Transition Metal Ions

在化学系化学结构、动力学和机制计划-A的支持下，马萨诸塞大学的里卡多·梅茨教授将研究过渡金属离子和金属簇离子如何与甲烷和乙烷反应，并将它们催化转化为更具工业用途的化学品。天然气主要是甲烷。在室温下，甲烷仍然是一种气体，即使在压力下也是如此。这限制了它作为交通燃料的用途。这些研究将着眼于将甲烷转化为更大的碳氢化合物所涉及的基本反应，这些碳氢化合物在室温下是液体，因此是更好的车辆燃料。这项工作的更广泛影响包括改进催化剂的潜在好处，以及培训研究生和本科生使用激光光谱学和质谱学等技术。最根本的是，从事这项研究的学生将吸收解决问题、实验设计、收集和分析数据以及交流结果的技能。梅茨教授还将通过尤里卡帮助向八年级女孩介绍科学研究！该奖项下正在进行的研究将使用各种技术来表征过渡金属离子和团簇离子与一个或多个甲烷或乙烷分子反应的反应物、中间体和产物。动力学研究的目标是测量反应的速度，并将反应性与离子的前线分子轨道的性质相关联。振动光谱将被用来鉴定反应产物和稳定的中间体。综上所述，这些研究有望有助于加深对过渡金属激活C-H键和C-C偶联机理的基础理解，最终目标是改进天然气中相对不活跃的主成分中C-H/C-C键的激活方法。金属-烷基离子的互补离子光碎片成像研究将被用来确定精确的共价键强度，测量光解离动力学，并检查自旋禁止过程。这一奖项反映了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。

WIth support from the Chemical Structure, Dynamics, and Mechanisms Program-A of the Chemistry Division, Professor Ricardo Metz of the University of Massachusetts, Amherst will study how transition metal ions and metal cluster ions react with methane and ethane and catalyze their conversion to more industrially useful chemicals. Natural gas is mostly methane. At room temperature methane remains a gas, even under pressure. This limits its usefulness as a transportation fuel. These studies will look at the fundamental reactions involved in converting methane to larger hydrocarbons that are liquids at room temperature and thus are better fuels for vehicles. The broader impacts of this work include potential benefits from improved catalysts as well as training graduate and undergraduate students in techniques such as laser spectroscopy and mass spectrometry. Most fundamentally, students engaged in this research will assimilate skills in problem solving, experimental design, the collection and analysis of data, and in communicating their results. Professor Metz will also help to introduce eighth-grade girls to science research through the Eureka! program.The research studies being conducted under this award will use a variety of techniques to characterize the reactants, intermediates and products of the reactions of transition metal ions and cluster ions with one or more methane or ethane molecules. Kinetics studies are targeted at measuring the rates of the reactions and correlating reactivity with properties of the frontier molecular orbitals of the ions. Vibrational spectroscopy will be employed to identify both reaction products and stable intermediates. Taken together, these studies are expected to contribute to enhanced fundamental understanding of the mechanisms of C-H bond activation and C-C coupling by transition metals, with the ultimate goal of improving methods for C-H/C-C bond activation in relatively unreactive principal components of natural gas streams. Complementary ion photofragment imaging studies of metal-alkyl ions will be utilized to determine precise covalent bond strengths, measure photodissociation dynamics and to examine spin-forbidden processes.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.