Preparation and NH3-SCR catalytic performance of CeTiOx catalysts with different pore structures
谭晨晨韩宇轩胡亚琴沈凯丁世鹏张亚平
TAN Chenchen;HAN Yuxuan;HU Yaqin;SHEN Kai;DING Shipeng;ZHANG Yaping
东南大学能源与环境学院能源热转换及其过程测控教育部重点实验室
为探究催化剂的孔结构对催化剂脱硝活性的影响,采用溶胶凝胶法分别制备了三维有序大孔-介孔(3DOM-m) CeTiOx、三维有序大孔(3DOM) CeTiOx、三维有序介孔(3DOm) CeTiOx及无序孔(DM) CeTiOx等四种不同孔结构的催化剂。NH3-SCR测试结果表明,催化剂活性依次为3DOM-m CeTiOx>3DOm CeTiOx>3DOM CeTiOx>DM CeTiOx,3DOM-m CeTiOx表现出更优异的催化活性,NO转化率在60000 h−1、250–400 ℃时超过90%。通过XRD、SEM、BET、NH3-TPD、in-situ DRIFTS等技术对催化剂进行表征分析。结果表明,催化剂的比表面积并不是决定CeTiOx脱硝活性的主导因素。3DOM-m CeTiOx具有高度有序的大孔-介孔结构、丰富的Brønsted酸酸性位点,进而提高了催化剂的脱硝活性。3DOM-m CeTiOx催化剂在NH3-SCR反应过程中同时遵循E-R机理和L-H机理。
To investigate the influence of pore structure on the catalytic activity of catalysts, four catalysts including three-dimensionally ordered macroporous-mesoporous (3DOM-m) CeTiOx, three-dimensionally ordered macroporous (3DOM) CeTiOx, three-dimensionally ordered mesoporous (3DOm) CeTiOx and disordered mesoporous (DM) CeTiOx were synthesized by the sol-gel method. The NH3-SCR denitration testing results show that the performance of the catalysts with different pore structures follows the sequence of 3DOM-m CeTiOx>3DOm CeTiOx>3DOM CeTiOx>DM CeTiOx, and the 3DOM-m CeTiOx shows an excellent catalytic activity, with more than 90% NO conversion in the range of 250–400 ℃ at a GHSV of 60000 h−1 . The characterization of catalysts by XRD, SEM, BET, NH3-TPD and in-situ DRIFTS indicates that the surface area is not the dominant factor determining the catalytic activity of CeTiOx. 3DOM-m CeTiOx has a highly ordered macroporous-mesoporous structure and abundant Bronsted acidic sites, thereby improving the denitrification activity. The NH3-SCR reaction over the 3DOM-m CeTiOx mainly follows the L-H and E-R mechanisms.
CeTiOx三维有序大孔有序介孔NH3-SCR脱硝
CeTiOx;3DOM structure;ordered mesoporous structure;NH3-SCR
主办单位:煤炭科学研究总院有限公司 中国煤炭学会学术期刊工作委员会