Catalytic Performance of NO Reduction by CO over Activated Semicoke Supported Fe/Co Catalysts

催化作用 氧气 化学 碳纤维 还原剂 氧化还原 金属 无机化学 活性炭 极限氧浓度 选择性还原 化学工程 材料科学 吸附 有机化学 复合材料 工程类 复合数
作者
Xingxing Cheng,Luyuan Wang,Zhiqiang Wang,Mengze Zhang,Chunyuan Ma
出处
期刊:Industrial & Engineering Chemistry Research [American Chemical Society]
卷期号:55 (50): 12710-12722 被引量:61
标识
DOI:10.1021/acs.iecr.6b00804
摘要

Performance of NO reduction by CO is studied over activated semicoke supported Fe/Co catalysts (FeCo/ASC). The influence of oxygen and CO concentration is investigated systematically. It is found that excess CO, with a CO:NO ratio greater than 2:1, could significantly enhance NO reduction, but oxygen, even with a concentration less than 1%, could strongly inhibit NO conversion efficiency due to the oxidation of active surface metal sites. To explore the role of CO in NO reduction, reactions without CO addition are also conducted. By comparing NO reduction behavior in the presence and absence of CO, it is found that carbon support is the main reducing agent if oxygen is in great excess, even when CO is provided. At the same time, NO reduction efficiency increases at higher oxygen concentration due to the increase of surface oxygen complex. However, excess oxygen is strongly undesired because serious gasification of carbon support is inevitable. But if oxygen concentration is not very high, CO could be fed in excess to consume oxygen and excellent NO reduction could be achieved. Possible reactions over the FeCo/ASC catalyst are summarized and the onset temperatures of each reaction are also listed to figure out possible reaction condition for NO reduction. It is observed that a temperature around 200 to 250 °C is favorable for NO reduction by CO in the presence of oxygen because reactions relevant to CO are already active but reactions for carbon support gasification are not activated yet. A reaction mechanism is also proposed, providing some insights on the complex catalytic reactions among NO, O2, CO, and carbon.
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