摘要
介孔分子筛具有较高比表面积、孔道结构规则及易于调节、热稳定性和水热稳定性较好、表面易改性等优点,在催化化学和吸附分离等领域有很大的潜在应用前景。本论文用SBA-15作为载体合成了M／SBA-15(Cu,Cr,Fe)和M-Al／SBA-15(Cu,Cr,Fe),在固定床微型反应器上考察了它们以CO或C3H6为还原剂时的deNOx性能。并用X-射线衍射、N2吸脱附、透射电镜、程序升温还原、X光电子能谱、傅立叶红外光谱、27Al魔角旋转固体核磁共振谱对其进行了表征
结果表明：负载金属后的SBA-15分子筛仍然保持了高度有序的二维六方介孔结构,其比表面积、孔径略有减少,催化剂表面元素均以离子态的物种存在,所负载的活性金属组分在SBA-15分子筛表面具有较高的分散度；以CO为还原剂时,M-Al／SBA-15(Cu,Cr,Fe)的deNOx活性高于M／SBA-15(Cu,Cr,Fe),并且其催化活性的顺序是Cr系>Cu系>Fe系。以C3H6为还原剂时,骨架中的Al的引入,使得Cu系催化剂活性增强,而Cr系和Fe系由于活性物质相互覆盖,活性大大降低。
The mesoporpous molecular sieve SBA-15 has been received much attention in fields of catalytic chemistry and asorption-separation,due to the asvantages of high surface area, ordered and tunable pore stucture, high thermal and hydwthermal stability and facile modification of surface properties.In this thesis,M/SBA-15 and M-Al/SBA-15(M=Cu,Cr,Fe) have been prepared by incipient wetness impregnation method.The performance of these samples in deNOx reaction with CO or C3H6 as reducing agent has been investigated by using a fixed bed reactor. XRD, BET, TEM,XPS,FT-IR,27Al MAS NMR are uesd to characterize these sample.
The results show that the hexagonal p6mm mesostructure of parent siliceous SBA-15 is maintained very well in M/SBA-15(M=Cu,Cr, Fe) and M-Al/SBA-15(Cu,Cr,Fe),BET surface area and the averge pore diameter decreased and the surfacial elements of the catalysts existed in the form of ion.The catalytic activity of the catalysts depended on the loading of M(Cu,Cr, Fe).In NO+CO reaction,M-Al/SBA-15(Cu,Cr,Fe) are much better than M/SBA-15(M=Cu,Cr, Fe),and series of Cr catalyst and better performance than series of Cu and series of Fe.
引文
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