This study was aimed to investigate the effects of hydrothermal aging, propene and SO<sub>2</sub> poisoning on the ammonia-selective catalytic reduction (NH<sub>3</sub>-SCR) performance of both...This study was aimed to investigate the effects of hydrothermal aging, propene and SO<sub>2</sub> poisoning on the ammonia-selective catalytic reduction (NH<sub>3</sub>-SCR) performance of both Cu-SAPO-34 and Cu-ZSM-5. The catalytic activities of fresh, aged and poisoned samples were tested in ammonia-selective catalytic reduction (NH<sub>3</sub>-SCR) of NO<sub>x</sub> conditions. The XRD, TG and N<sub>2</sub>-desorption results showed that the structures of the Cu-SAPO-34 and Cu-ZSM-5 remained intact after 750˚C hydrothermally aged, SO<sub>2</sub> and propene poisoned. After hydrothermal aging at 750˚C for 12 h, the NO reduction performance of Cu-ZSM-5 was significantly reduced at lower temperatures, while that of Cu-SAPO-34 was less affected. Moreover, Cu-SAPO-34 catalyst showed high NO conversion with SO<sub>2</sub> or propene compared to Cu-ZSM-5. However, Cu-ZSM-5 showed a larger drop in catalytic activity with SO<sub>2</sub> or propene compared to Cu-SAPO-34 catalyst. The H<sub>2</sub>-TPR results showed that Cu<sup>2 </sup> ions could be reduced to Cu<sup> </sup> and Cu<sup>0</sup> for Cu-ZSM-5, while no significant transformation of copper species was observed for Cu-SAPO-34. Meanwhile, the UV-vis DRS results showed that CuO species were formed in Cu-ZSM-5, while little changes were observed for the Cu-SAPO-34. Cu-SAPO-34 showed high sulfur and hydrocarbon poison resistance compared to Cu-ZSM-5. In summary, Cu-SAPO-34 with small-pore zeolite showed higher hydrothermal stability and better hydrocarbon and sulfur poison resistant than Cu-ZSM-5 with medium-pore.展开更多
运用 AES,XPS,XRD和 TEM等手段研究了 La Co O3模型催化剂 SO2 中毒过程表面化学状态、晶相结构及表面形貌的变化状况 ,初步推断了 La Co O3钙钛矿型复合金属氧化物催化剂的 SO2 中毒机理 .在 SO2强化中毒过程中 ,SO2 与催化剂的活性组...运用 AES,XPS,XRD和 TEM等手段研究了 La Co O3模型催化剂 SO2 中毒过程表面化学状态、晶相结构及表面形貌的变化状况 ,初步推断了 La Co O3钙钛矿型复合金属氧化物催化剂的 SO2 中毒机理 .在 SO2强化中毒过程中 ,SO2 与催化剂的活性组分 La Co O3反应生成硫酸镧和氧化亚钴 ,而在催化剂膜层内部则生成硫酸镧、亚硫酸镧及氧化亚钴 . SO2 对活性组分层的侵入及硫与 La Co O3活性组分的反应破坏了催化剂的钙钛矿结构 ,使得催化剂彻底中毒 .当中毒温度较低及中毒时间较短时 ,硫在膜层中呈峰形分布 ,其浓度随中毒温度及时间的增加而增加 .随中毒温度的升高及中毒时间的增长 ,由于亚硫酸盐的分解作用 ,S在活性层中的浓度反而降低 ,中毒深度则继续增加 .展开更多
文摘This study was aimed to investigate the effects of hydrothermal aging, propene and SO<sub>2</sub> poisoning on the ammonia-selective catalytic reduction (NH<sub>3</sub>-SCR) performance of both Cu-SAPO-34 and Cu-ZSM-5. The catalytic activities of fresh, aged and poisoned samples were tested in ammonia-selective catalytic reduction (NH<sub>3</sub>-SCR) of NO<sub>x</sub> conditions. The XRD, TG and N<sub>2</sub>-desorption results showed that the structures of the Cu-SAPO-34 and Cu-ZSM-5 remained intact after 750˚C hydrothermally aged, SO<sub>2</sub> and propene poisoned. After hydrothermal aging at 750˚C for 12 h, the NO reduction performance of Cu-ZSM-5 was significantly reduced at lower temperatures, while that of Cu-SAPO-34 was less affected. Moreover, Cu-SAPO-34 catalyst showed high NO conversion with SO<sub>2</sub> or propene compared to Cu-ZSM-5. However, Cu-ZSM-5 showed a larger drop in catalytic activity with SO<sub>2</sub> or propene compared to Cu-SAPO-34 catalyst. The H<sub>2</sub>-TPR results showed that Cu<sup>2 </sup> ions could be reduced to Cu<sup> </sup> and Cu<sup>0</sup> for Cu-ZSM-5, while no significant transformation of copper species was observed for Cu-SAPO-34. Meanwhile, the UV-vis DRS results showed that CuO species were formed in Cu-ZSM-5, while little changes were observed for the Cu-SAPO-34. Cu-SAPO-34 showed high sulfur and hydrocarbon poison resistance compared to Cu-ZSM-5. In summary, Cu-SAPO-34 with small-pore zeolite showed higher hydrothermal stability and better hydrocarbon and sulfur poison resistant than Cu-ZSM-5 with medium-pore.
文摘运用 AES,XPS,XRD和 TEM等手段研究了 La Co O3模型催化剂 SO2 中毒过程表面化学状态、晶相结构及表面形貌的变化状况 ,初步推断了 La Co O3钙钛矿型复合金属氧化物催化剂的 SO2 中毒机理 .在 SO2强化中毒过程中 ,SO2 与催化剂的活性组分 La Co O3反应生成硫酸镧和氧化亚钴 ,而在催化剂膜层内部则生成硫酸镧、亚硫酸镧及氧化亚钴 . SO2 对活性组分层的侵入及硫与 La Co O3活性组分的反应破坏了催化剂的钙钛矿结构 ,使得催化剂彻底中毒 .当中毒温度较低及中毒时间较短时 ,硫在膜层中呈峰形分布 ,其浓度随中毒温度及时间的增加而增加 .随中毒温度的升高及中毒时间的增长 ,由于亚硫酸盐的分解作用 ,S在活性层中的浓度反而降低 ,中毒深度则继续增加 .
