High Activity Catalytic Redox Sites Within Zeolites

提案标题：沸石中的高活性催化氧化还原位点提案编号：CTS-0099359主要研究者：Carl Lund机构：纽约州立大学布法罗分校本提案的目的是确定沸石催化剂上高活性氧化还原位点的化学性质。 在以前的工作中，PI提出了新的假设，即阴离子，而不是阳离子，参与氧化还原活性。 提出了一个涉及硝酸盐和亚硝酸盐物种的动力学模型来解释反应物在一定分压以上的反常行为。 具体地，发现当分压超过临界值时，一氧化二氮在沸石催化剂上的分解速率跳到更高的水平。 因为这种现象只发生在沸石与铁离子交换后，与阳离子有一定的相互作用。拟议的研究可能揭示一种新型的氧化还原化学，可应用于NOx化合物的分解以及部分氧化反应。 使用重量法，红外光谱，微量热法，同位素标记的研究，和详细的动力学研究可能会揭示的性质和身份的高活性氧化还原位点。 这项工作有可能阐明在工业和环境应用中的重要现象，包括氮氧化物的选择性催化还原。

Proposal Title: High Activity Catalytic Redox Sites within ZeolitesProposal Number: CTS-0099359Principal Investigator: Carl LundInstitution: State University of New York at BuffaloThe objective of this proposal is to determine the chemical nature of high activity redox sites on zeolite catalysts. In previous work the PI postulated the novel hypothesis that the anions, rather than the cations, were involved the redox activity. A kinetic model involving nitrate and nitrite species was proposed to explain anomalous behavior above a certain partial pressure of reactant. Specifically, it was found that the rate of decomposition of nitrous oxide over a zeolite catalyst jumped to a higher level when its partial pressure exceeded a critical value. Because this phenomenon only occurred when the zeolite had been ion-exchange with iron, there is some interaction with the cation. The proposed research may reveal a new type of redox chemistry, which may be applied to the decomposition of NOx compounds as well as partial oxidation reactions. The use of gravimetry, infrared spectroscopy, microcalorimetry, isotope-labeling studies, and detailed kinetic studies may reveal the nature and identity of the high activity redox sites. This work has the potential to elucidate phenomena important in industrial and environmental applications including the selective catalytic reduction of nitrogen oxides.