载体不同焙烧温度对NSR催化剂Pt-K2CO3/K2Ti8O17中碳酸盐的状态和储存性能的影响
Effect of Support Calcination Temperature on the States and Storage Property of Carbonates in NOx Storage and Reduction Catalyst Pt-K2CO3/K2Ti8O17
采用浸渍法合成了一系列载体焙烧温度不同的负载型碳酸盐基NSR催化剂Pt-K2CO3/K2Ti8O17。NOx储存还原测试结果表明:催化剂的活性与载体的焙烧温度有很大关系。载体焙烧温度为350℃的催化剂拥有最大的比表面积(211 m2/g),最高的NOx储存量(0.68mmol/g)及最高的NOx还原消除效率(99.1%)。通过计算,该催化剂中K的利用率高达94.4%。XRD,SEM,NH3-TPD和CO2-TPD等表征结果显示:焙烧温度超过650℃时,载体K2Ti8O17分解为K2Ti6O13 与TiO2,使得载体比表面积,形貌,酸碱性以及K物种的分布发生明显变化,从而引起储存量的差异。催化剂中K物种的存在形式有 K2O, -OK,表面碳酸盐及体相碳酸盐,相对含量随载体焙烧温度变化而变化,其中表面碳酸盐是最有利于NOx储存的活性物种。 In-situ DRIFTS结果表明,单齿硝酸盐和单齿亚硝酸盐是主要的NOx储存物种
series of carbonate based NOx storage and reduction catalysts Pt-K2CO3/K2Ti8O17 with the support calcined at different temperatures were synthesized by sequential impregnation. The results of NOx storage and reduction show that the catalytic activity of these catalysts depends strongly on the calcination temperature of support. The catalyst with its support calcined at 350℃ possesses the largest BET specific surface area (211 m2/g), the highest NOx storage capacity (0.68 mmol/g) and the highest NOx reduction percentage (99.1%). The utilization efficiency of K species in this catalyst is as high as 94.4%. Based upon multiple characterizations, such as XRD, SEM, NH3-TPD and CO2-TPD, it is found that the calcination over 650℃ can cause the decomposition of K2Ti8O17 to K2Ti6O13 and TiO2, making the specific surface areas, morphology, acid-base properties of the support and the distribution of K species obviously different, which further influences the NOx storage capacity. It is also revealed that the K species exist in several forms including K2O, -OK groups, surface potassium carbonate and bulk or bulk-like potassium carbonate, which have different stability. The relative concentrations of these species vary with support calcination temperature, among them the surface carbonate species are identified as the most favorable species to NOx storage. In-situ DRIFTS results indicate that monodentate nitrates and monodentate nitrites are the dominant NOx storage species.
孟明、张玉霞
金属元素无机化合物化学工业精细化学工业
氮氧化物储存还原钛酸盐碳酸盐焙烧温度
nitrogen oxidesstorage and reductiontitanatecarbonatecalcination temperature
孟明,张玉霞.载体不同焙烧温度对NSR催化剂Pt-K2CO3/K2Ti8O17中碳酸盐的状态和储存性能的影响[EB/OL].(2014-04-08)[2025-08-16].http://www.paper.edu.cn/releasepaper/content/201404-93.点此复制
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