Spectroscopic Elucidation of Cu and Fe Active Sites in Zeolites

甲烷是迄今为止天然气的最大组成部分，是最丰富的化石燃料资源之一，但由于运输液化天然气的成本和危险，它仍然没有得到充分利用。 这个问题可以通过将甲烷转化为甲醇来解决，甲醇是一种环境友好的液体燃料，已被确定为天然气在运输部门最有前途的应用。 然而，目前使用的工业规模甲烷/甲醇转化是能量密集型的，需要在高温和高压下的多个步骤来克服甲烷固有的低反应性。 为了使从天然气衍生的甲醇燃料具有成本效益，需要更有效的方法。 在化学系化学催化项目的资助下，斯坦福大学的所罗门教授正在研究一类称为沸石的材料，它们可以进行这种具有挑战性的化学反应。 所罗门教授的研究揭示了这些材料在分子水平上是如何运作的。 这种见解对于理解如何设计用于甲烷/甲醇转化以及其他经济上重要的反应的改进催化剂是重要的。 所罗门教授的研究还与斯坦福大学周边地区为K-12学生提供服务的外展活动相结合。 这包括开发一个影子计划，使高中生在体验研究实验室在斯坦福大学。该项目建立在教授所罗门的铁和铜沸石，包括他们的几何/电子结构，在选择性烃氧化反应，以及它们的相关性，铁和铜酶的光谱和计算研究。它还将这种努力扩展到对NOx污染物进行选择性催化还原（SCR）的金属沸石。这些研究提供了对反应机制的详细了解，定义了活性位点形成的结构贡献以及反应性的一般原理。由此产生的洞察力可能会导致改进的催化剂，用于许多具有经济意义的化学转化，包括天然气转化为CH 3OH燃料，以及减少柴油发动机产生的NOx污染物。这项建议涉及重大的国际合作，所罗门教授参与了一些方向，以提高物理无机化学和光谱学的知识。所罗门教授的团队还在与当地K-12学校的外联活动中发挥了领导作用，包括开发一个影子项目，让高中生体验斯坦福大学的研究实验室。

Methane, by far the largest component of natural gas, is one of the most abundant fossil fuel resources, but it remains underutilized due to costs and dangers associated with transporting liquefied natural gas. This problem could be resolved by converting methane into methanol, an environmentally friendly liquid fuel that has been identified as the most promising application for natural gas in the transportation sector. The industrial-scale methane/methanol conversion in use today is energy intensive, however, requiring multiple steps at high temperatures and pressures to overcome the inherently low reactivity of methane. For methanol fuel derived from natural gas to be cost-effective, a more efficient method is required. With funding from the Chemical Catalysis Program of the Chemistry Division, Professor Solomon of Stanford University is studying a class of materials called zeolites that perform this challenging chemistry. Professor Solomon's research is revealing how these materials operate on the molecular level. This insight is important for understanding how to design improved catalysts for methane/methanol conversion, as well as other economically significant reactions. Professor Solomon's research is also coupled to outreach activities that serve K-12 students in the areas surrounding Stanford University. This includes developing a shadowing program that brings high school students in to experience research laboratories at Stanford.This project builds on Professor Solomon's current spectroscopic and computational studies of Fe and Cu zeolites, including their geometric/electronic structures, reactivity in selective hydrocarbon oxidation, and their correlation to Fe and Cu enzymes. It also extends this effort to metallozeolites that perform selective catalytic reduction (SCR) of NOx pollutants. These studies are providing detailed insight into reaction mechanisms, defining structural contributions to active site formation, as well as general principles of reactivity. The resulting insight may lead to improved catalysts for a number of economically significant chemical transformations, including the conversion of natural gas to CH3OH fuel, and the abatement of NOx pollutants generated by diesel engines. This proposal involves significant international collaboration, and Professor Solomon is involved in a number of directions to enhance knowledge in physical inorganic chemistry and spectroscopy. Professor Solomon's group has also taken a leadership role in outreach to local K-12 schools, including developing a shadowing program that brings high school students in to experience research laboratories at Stanford.