RUI: Investigating the Influence of Halogen Ligands on the Ability of Late Gas-Phase Transition Metal Ions to Activate Bonds in Small Substrate Molecules

在该项目中，阿肯色州中部大学的William Taylor教授和他的本科生研究小组正在研究小分子和离子之间的反应，这些小分子和离子都含有卤素元素的原子（卤素包括氟、氯、溴和碘）。离子含有过渡金属元素（例如铜、镍或金）。 当今许多重要的工业过程涉及含有过渡金属原子的催化剂。 因此，泰勒教授实验室的研究为更广泛的催化领域提供了信息，这是估计90%的化学产品生产的关键部分。 催化工艺通过直接补救污染物或减少工业化学品生产的环境负担而具有切实的环境效益。参与这项工作的本科生将受益于宝贵的研究经验，提高科学领域的保留率，并为各种职业选择做好准备。该项目探讨了通过配体环境对中性分子中键活化的金属中心的电子修饰的影响。本项目中的研究探讨了MX+（M=Ni、Cu、Au; X=F、Cl、Br、I）与一些已知是强效温室气体和臭氧消耗物质的卤代化合物的化学性质。此外，CuX+和AuX+（X=Cl，F）与甲烷的反应进行检查，以探索低能量的过程，导致这种丰富的，但相对惰性的化学资源的功能化。所有的反应进行了实验研究，在气相中使用选定的离子漂移池反应器，产生过渡金属离子在溅射辉光放电源。然后，通过添加所需的卤素对这些金属离子进行化学改性，选择质量，并将其引入含有感兴趣的中性反应物分子的漂移池中。 使用第二个四极杆进行反应产物的分析。实验结果补充计算与密度泛函计算和MP2理论获得额外的见解可能的反应机制。

In this project supported by the Chemical Structure, Dynamics and Mechanisms Program of the Division of Chemistry, Professor William Taylor of the University of Central Arkansas and his undergraduate research team are studying reactions between small molecules and ions which both contain atoms of halogen elements (the halogens include fluorine, chlorine, bromine and iodine). The ions contain transition metal elements (for example copper, nickel or gold). Many important industrial processes today involve catalysts that contain transition metal atoms. The studies in Professor Taylor's laboratory thus inform the broader area of catalysis, which is a key part of the production of an estimated 90% of all chemical products. Catalytic processes have a tangible environmental benefit by either direct remediation of pollutants or by reducing the environmental burden of industrial chemical production. Undergraduates participating in this work benefit from a valuable research experience that increases retention rates in the sciences, and prepares them for a variety of career choices.The project explores the influence of electronic modifications to metal centers via the ligand environment on bond activation in neutral molecules. Studies addressed in this project examine the chemistry of MX+ (M=Ni, Cu, Au; X=F, Cl, Br, I) with a number of halogenated compounds known to be potent greenhouse gases and ozone depleters. In addition, reactions of CuX+ and AuX+ (X=Cl, F) with methane are examined in order to explore low-energy processes leading to the functionalization of this abundant, yet relatively inert, chemical resource. All reactions are studied experimentally in the gas phase using a selected ion drift cell reactor which generates transition metal ions in a sputtering glow discharge source. These metal ions are then be chemically modified with the addition of the desired halogen, mass selected, and introduced into a drift cell containing the neutral reactant molecule of interest. Analysis of reaction products is carried out using a second quadrupole. Experimental results are complemented computationally with density functional calculations and MP2 theory to gain additional insights into possible reaction mechanisms.