Mechanistic Studies of TiO2-based Mn/Ni Catalysts for the Low Temperature SCR of NOx with NH3

自从氨选择性催化还原NO被公认为是环境保护的关键化学转化以来，中温脱氮工艺在世界范围内得到了广泛的应用。对于将用于加工替代燃料和化学原料的SCR催化剂来说，Hoewever、水和二氧化硫中毒是一个重要的挑战。首席研究人员之前的工作表明，Mn/Ti02在低至80oC的温度下具有活性，并且耐水。为了提高催化剂的抗二氧化硫能力，在催化剂中加入镍似乎是有希望的。这项研究将在关键的机理和光谱研究的基础上，对Mn-Ni/Ti02系统有一个基本的理解。将利用瞬变动力学方法对反应途径提供新的见解，并为高选择性奠定基础。首席研究人员还将使用先进的仪器能力，如标记化合物的原位FTIR光谱，以确定吸附物种和活性中间体。其他表面分析技术被巧妙地融入到拟议的工作中。这两种方法的结合是优秀的、现代催化研究的特征。这项研究的更广泛影响包括对学生进行先进催化和表征技术的教育，以及参与相关技术应用。学生将参与海报和论文演示，并准备大量出版物。首席研究员致力于为研究项目招募代表不足的少数族裔，包括与辛辛那提大学一个新的种族工程办公室合作。

Medium temperature DeNOx processes have been widely utilized throughout the world since the selective catalytic reduction (SCR) of NO by ammonia is widely recognized as a key chemical transformation for environmental protection. Hoewever, water and sulfur dioxide poisoning are important challenges for SCR catalysts that will be used to process alternative fuels and chemical feedstocks. Prior work by the principal investigator has demonstrated that Mn/TiO2 is active at temperatures as low as 80 oC and is resistant to water. Addition of Ni to this catalyst appears promising in order to enhance sulfur dioxide tolerance. The research will provide a fundamental understanding of Mn-Ni/TiO2 systems based on key mechanistic and spectroscopic investigations. Transient kinetic methods will be utilized in order to provide new insights into the reactions pathways and to establish the basis for high selectivity. The principal investigator will also use advanced instrumentation capabilities such as in situ FTIR spectroscopy with labeled compounds to determine adsorbed species and reactive intermediates. Other surface analysis techniques are skillfully incorporated into the proposed work. The combination of approaches is characteristic of excellent, modern catalysis research.The broader impacts of this research include education of students in advanced catalysis and characterization techniques and involvement in relevant technological applications. Students will be involved in poster and paper presentations and in preparation of numerous publications. The principal investigator is committed to recruiting under-represented minorities for the research program, including working with a new ethnic engineering office at the University of Cincinnati.