Fundamental Studies of the Oxidation of Oxidation of Sulfur Dioxide to Sulfur Trioxide over Supported Metal-Oxide Catalysts

CTS-9626893研究了负载型固体金属氧化物催化剂上二氧化硫氧化为三氧化硫的分子结构-活性关系。（硫酸接触工艺，使用支撑熔盐作为催化剂，不是本研究的主题。）解决的基本问题包括动力学，反应机制，活性位点的性质，包括大小和结构，以及载体，表面添加剂和各种气体（如水，一氧化氮，碳氢化合物和氨）的影响。合成了含有钒、钼、铬、铼或锰的可还原氧化物的模型支撑催化剂，用拉曼光谱、红外光谱和核磁共振光谱对其进行了表征，并测试了该反应的催化活性。这些信息用于建立二氧化硫氧化的构效关系。固体氧化物催化氧化二氧化硫在硫酸的工业生产中很重要，在一些环境技术中也很重要，包括从工业（包括发电机）工厂中去除氮和硫的DESONOX和SNOX工艺，以及去除氮氧化物的选择性催化还原，因为三氧化硫是一种毒药。

ABSTRACT CTS-9626893 This is a study of molecular structure-activity relationships in the oxidation of sulfur dioxide to sulfur trioxide over supported solid metal-oxide catalysts. (The sulfuric acid contact process, which uses a supported molten salt as the catalyst, is not the subject of this study.) Fundamental issues addressed include the kinetics, the reaction mechanism, the nature of the active site including size and structure, and the effects of the support, surface additives and various gases such as water, nitric oxide, hydrocarbons, and ammonia. Model supported catalysts containing reducible oxides of vanadium, molybdenum, chromium, rhenium, or manganese are synthesized, characterized by Raman, infrared, and nuclear magnetic resonance spectroscopies, and tested for catalytic activity for the subject reaction. This information is used to establish structure-activity relationships for oxidation of sulfur dioxide. The solid-oxide catalyzed oxidation of sulfur dioxide is important in the industrial production of sulfuric acid as well as in several environmental technologies including the DESONOX and SNOX processes for removing nitrogen and sulfur from industrial (including electric power generator) plants and selective catalytic reduction to remove nitrogen oxides, for in which sulfur trioxide is a poison.