Abstract

分别采用柠檬酸络合法、改性共沉淀法和湿浸渍法制备了掺Ba纳米ZrO2材料,负载Ru后用于催化氨合成反应.采用X射线衍射、CO2程序升温脱附(CO2-TPD)、N2物理低温吸附、H2程序升温还原技术(H2-TPR)、扫描电镜(SEM)、透射电镜(TEM)、X射线光电子能谱(XPS)和CO化学吸附对载体材料和催化剂进行了表征.结果表明,不同方法制备载体的物相结构和织构性能均有明显差别,负载Ru后催化剂的氨合成性能差别也较大.其中,以柠檬酸络合法制备的载体材料中Ba以BaZrO3的形式存在,钙钛矿型BaZrO3具有较强的供电子能力,电子可以通过Ru与载体间强相互作用传递到Ru表面,有效地促进N≡N的断裂,使催化剂的低温活性显著提高.在425℃,3 MPa,空速为10000 h-1条件下,出口氨浓度为5.72%.其氨合成活性分别是改性共沉淀法和湿浸渍法制备催化剂的3.8倍和14.3倍.

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