Role of Acid Sites in Selective Reduction of NO by Methane over PD-Based Catalysts in Presence of Excess Oxygen

摘要：提案题目：在过量氧存在下，酸性位点在Pd基催化剂上甲烷选择性还原NO中的作用提案号：cts9726465首席研究员Daniel E. Resasco机构：俄克拉何马大学教授Daniel E. Resasco将研究在酸性载体上Pd存在下甲烷选择性催化还原NO的各个方面。这项工作与各种环境问题相关：它为从燃烧气体中催化去除氮氧化物提供了新的科学见解，它导致了甲烷的利用，它导致了在更清洁（富氧）条件下燃烧燃料的可能性，因此，它允许更高的能源效率和每单位能源生产更少的二氧化碳产生。将追求三个目标：确定酸性位点在提供SCR选择性方面的作用，以支持或交换在沸石或硫酸氧化锆上支持的Pd；通过反应物或可能的中间体的红外光谱，以及同位素标记化合物的瞬态动力学，从动力学角度确定可能的反应机制；并研究钯催化剂在水和二氧化硫存在下的反应耐受性。Pd的状态将通过x射线吸收，温度程序还原，电子显微镜和探针分子的化学吸附来表征。酸性位点将通过微量热法、化学吸附和弱碱的程序升温解吸来表征。

ABSTRACT Proposal Title: Role of Acid Sites in the Selective Reduction of NO by Methane over Pd-Based Catalysts in the Presence of Excess Oxygen Proposal Number: CTS-9726465 Principal Investigator Daniel E. Resasco Institution: University of Oklahoma Professor Daniel E. Resasco, from the University of Oklahoma, will investigate various aspects of the selective catalytic reduction of NO with methane in the presence of oxygen, over Pd on acidic supports. This work is of relevance to various environmental concerns: it provides new scientific insights into the catalytic removal of NOx from gases of combustion, it leads to the utilization of methane, it leads to the possibility of burning fuels under leaner (oxygen-rich) conditions, and as a consequence, it allows higher energy efficiency and less generation of CO2 per unit of energy production. Three objectives will be pursued: to determine the role of acidic sites in providing SCR selectivity to Pd supported or exchanged in zeolites or supported on sulfated zirconia; to determine the possible reaction mechanisms kinetically, by infrared spectroscopy of reactants or possible intermediates, and by transient kinetics of isotopically labeled compounds; and to investigate the tolerance of the Pd catalysts during reaction in the presence of water and SO2. The state of Pd will be characterized by x-ray absorption, temperature programmed reduction, electron microscopy, and chemisorption of probe molecules. The acidic sites will be characterized by microcalorimetry and by chemisorption and temperature programmed desorption of weak bases.