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华东理工大学学报(自然科学版):2018,44(5):699-706
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制备方法对双金属Fe-Cu-ZSM-5催化剂的NH3-SCR反应性能的影响
(华东理工大学工业催化研究所, 上海 200237)
Effect of Preparation Method on Catalytic Performance of Fe-Cu-ZSM-5 for Selective Catalytic Reduction of NOx by NH3
(Research Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai 200237, China)
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投稿时间:2017-08-30    
中文摘要: 采用不同方法制备了双金属改性Fe-Cu-ZSM-5催化剂,结果发现用等体积浸渍法制备的Fe0.7-Cu0.97-ZSM-5(IWI)催化剂活性最高,而用液相离子交换法制备的Fe0.59-Cu1.0-ZSM-5(IE)催化剂活性稍逊于Fe0.7-Cu0.97-ZSM-5(IWI),但显著优于采用先离子交换后浸渍法制备的Fe0.65(IWI)-Cu0.95(IE)-ZSM-5催化剂。结果表明:用不同方法制备的Fe-Cu-ZSM-5催化剂中,活性金属Cu和Fe物种的存在状态、催化剂的可还原性和NO氧化能力以及催化剂表面的酸性等因素是影响催化剂SCR活性的关键因素。
Abstract:Nitrogen oxides is one of the major pollutants in diesel exhaust, which has caused serious environmental pollution. The selective catalytic reduction (SCR) is the most efficient way to control NOx emission, and the key is the catalysts with high activity. Recently, zeolites-based catalysts have been attracted more attention because of their special pore structure and catalytic performance. In this paper, impregnation, liquid-state ion exchange, and liquid-state ion exchange followed by impregnation methods were employed to prepare Fe-Cu-ZSM-5 catalyst. Over 80% of NO conversion can be achieved at the temperature region of 188-530℃, 200-520℃, and 240-530℃ for catalyst Fe0.7-Cu0.97-ZSM-5(IWI), Fe0.59-Cu1.0-ZSM-5(IE) and Fe0.65(IWI)-Cu0.95(IE)-ZSM-5, respectively. It was found that the catalyst Fe0.7-Cu0.97-ZSM-5 prepared with impregnation method exhibited the best catalytic performance for SCR reaction. However, the Fe0.65-Cu0.95-ZSM-5 catalyst prepared with liquid-state ion exchange followed by impregnation exhibited the lowest catalytic performance. The catalysts were characterized by XRD, UV-vis, H2-TPR, XPS, NH3-TPD, and NO oxidation. It was revealed that the catalyst Fe0.7-Cu0.97-ZSM-5(IWI) had more isolated Cu2+ and Fe3+ species at the exchange site, which are the active species for NH3-SCR reaction at the low-temperature region. In addition, the catalyst Fe0.7-Cu0.97-ZSM-5(IWI) had the stronger redox ability and NO oxidation ability, as well as more acid sites on catalyst surface compared with catalyst Fe0.59-Cu1.0-ZSM-5(IE) and Fe0.65 (IWI)-Cu0.95 (IE)-ZSM-5. Above all, the states of active Cu and Fe species, reducibility of the catalyst and acidic properties on the catalyst surface are the critical factors for the catalytic performance of the Fe-Cu-ZSM-5 catalysts.
文章编号:     中图分类号:TQ032    文献标志码:
基金项目:国家自然科学基金面上项目(21577034)
引用本文:
焦云磊,陈艺元,郭杨龙,郭耘,卢冠忠,詹望成.制备方法对双金属Fe-Cu-ZSM-5催化剂的NH3-SCR反应性能的影响[J].华东理工大学学报(自然科学版),DOI:10.14135/j.cnki.1006-3080.20170830001.

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