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铈基过渡金属复合氧化物上氨催化还原NOx的构效关系
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Abstract:
采用共沉淀法制备了一系列铈基过渡金属复合氧化物催化剂，通过催化活性评价和催化表征考察了铈基过渡金属复合氧化物催化还原NOx的构效关系。研究表明：铈基过渡金属复合氧化物催化剂活性为4Ce1Ni > 4Ce1Mn > 4Ce1Cu > CeO2 > 4Ce1Cr。4Ce1Ni催化剂在325℃时NOx最大转化率可达92%，同时其具有良好的抗水性。铈基过渡金属复合氧化物催化剂的活性与其物化结构、表面活性氧物种比值和过渡金属活性组分的形态有关。催化剂的比表面积和Olatt/Oads比值大小均为4Ce1Ni > 4Ce1Mn > 4Ce1Cu > CeO2 > 4Ce1Cr，与催化活性成正相关性。4Ce1Ni、4Ce1Mn、4Ce1Cu、CeO2和4Ce1Cr催化剂中活性组分分别为Ni2+、Mn3+和Mn4+、Cu2+和Cr6+，其中Ni2+的催化活性最强，Mn3+和Mn4+次之。
Series of composite oxides containing Ce and transition metal were prepared by coprecipitation method. Relationship of structure-activity for catalytic reduction of NOx by NH3 on composite oxides containing Ce and transition metal was investigated by activity test and catalyst characterization. It shows that NOx conversion over catalysts decreased in the order of 4Ce1Ni > 4Ce1Mn > 4Ce1Cu > CeO2 > 4Ce1Cr. 4Ce1Ni with good water tolerance exhibits the highest NOx conversion of 92% at 325？C. The activity of composite oxides containing Ce and transition metal catalysts is related to their physico-chemical structure, active oxygen species and active sites of transition metal. Both surface area and the ratio of Olatt/Oads decreased in the order of 4Ce1Ni > 4Ce1Mn > 4Ce1Cu > CeO2 > 4Ce1Cr, which showed positive correlation with activity. The active components of 4Ce1Ni, 4Ce1Mn, 4Ce1Cu, CeO2 and 4Ce1Cr, are Ni2+, Mn3+ and Mn4+, Cu2+ and Cr6+ respectively. The catalytic activity of Ni2+ is the highest, followed by 3+ and Mn4+.
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