基于助剂存在形式的变化研究Ru/C氨合成催化剂失活机理

项目名称： 基于助剂存在形式的变化研究Ru/C氨合成催化剂失活机理

项目编号： No.21203028

项目类型： 青年科学基金项目

立项/批准年度： 2013

项目学科： 物理化学

项目作者： 林炳裕

作者单位： 福州大学

项目金额： 25万元

中文摘要： 钌催化剂是继铁催化剂之后的新一代氨合成催化剂，其中以活性炭为载体的钌催化剂最有应用前景，而炭载体的甲烷化流失是其工业化应用的最主要障碍。但是现有研究表明活性炭载体的初始甲烷化温度高于理想的工业氨合成反应所需要的温度。我们最新研究发现低温长时间氨合成反应前后钌催化剂中K和Ba助剂的存在形式不同，并且K助剂与活性炭载体之间存在反应。本项目提出Ru/C催化剂中助剂存在形式的变化可能是造成催化剂失活的重要因素，将考察催化剂活化及氨合成反应过程中助剂的存在形式、生成路径及其相关影响因素；详细表征氢、氮和氨分子在催化剂表面的吸附行为和化学状态；并结合催化剂的其它物化性质及氨合成性能评价结果来分析钌催化剂的内在本质，阐明催化剂的失活机理。本研究将有助于认识和解决催化剂的稳定性问题，为制备高效钌系氨合成催化剂提供理论依据和指导，并为炭材料为载体的各种负载型催化剂的开发奠定了理论基础。

中文关键词： 氨合成；Ru/C；失活；助剂；

英文摘要： Ruthenium catalyst has been recognized as the second generation catalyst for ammonia synthesis. It was found Ru catalyst supported on activated carbon was the most promising candidates for the commercialization of Ru catalyst, and the methanation of carbon support was a major hurdle. However, the formation temperatures of methane for Ru/C catalysts were higher than the reaction temperatures used in industrial ammonia synthesis. Previously, we found the presence of reaction between KOH and activated carbon, furthermore, the existing form of K and Ba promoters before and after long-term ammonia synthesis test were different. Based on these new finds, this project proposed the change in the existing form of promoters should be an important factor for the deactivation of Ru/C catalysts. In this project, we will systemically investigate the existing form of promoters, the reaction way and the influence factors during catalyst activation or ammonia synthesis. The adsorption behavior and chemical state of hydrogen, nitrogen and ammonia molecule on Ru/C catalysts will also be characterized. Furthermore, the other physico-chemical properties, the ammonia synthesis activity and the stability of Ru catalyst will also be evaluated. Therefore, we can learn the essence of ruthenium catalyst, and the deactivation mechanism of

英文关键词： Ammonia synthesis；Ru/C；Deactivation；Promoter；