化工学报
化工學報
화공학보
CIESC Jorunal
2015年
10期
3903-3910
,共8页
王龙飞%张亚平%郭婉秋%沈凯%郑鹏飞%杨林军
王龍飛%張亞平%郭婉鞦%瀋凱%鄭鵬飛%楊林軍
왕룡비%장아평%곽완추%침개%정붕비%양림군
催化剂%载体%原位氨气吸附漫反射红外%三氧化钨%活化
催化劑%載體%原位氨氣吸附漫反射紅外%三氧化鎢%活化
최화제%재체%원위안기흡부만반사홍외%삼양화오%활화
catalyst%support%in situ DRIFTS analysis of NH3 adsorption%tungsten%activation
采用共沉淀法制备了WO3/TiO2-ZrO2脱硝催化剂,并用固定床反应器进行活性评价,采用BET、XRD、TPD、氨气吸附漫反射FT-IR进行表征。结果显示,ZrO2掺杂增强了TiO2的Lewis酸性;负载WO3之后,位于3.1~1.7 nm之间孔隙的稳定性显著增强;NH3的吸附与活化分别由TiO2-ZrO2载体和WO3完成;WO3中W元素强大的电负性,促进了NH3的N—H键由共价键向离子键过渡,进而导致了NH3的活化。脱硝活性结果显示:当WO3含量为9%(质量)时,催化剂脱硝活性最高,并在320~420℃的温度窗口保持94%以上。(9%)WO3/TiO2-ZrO2具有更加稳定的孔隙结构(4.4~1.7 nm),表面Br?nsted酸中心数量增加,Lewis酸中心的强度和酸量增加的幅度最大, NH3-SCR过程中的活性中间产物NH2的吸收峰更加明显,这些特征可能是其脱硝活性最好的原因。
採用共沉澱法製備瞭WO3/TiO2-ZrO2脫硝催化劑,併用固定床反應器進行活性評價,採用BET、XRD、TPD、氨氣吸附漫反射FT-IR進行錶徵。結果顯示,ZrO2摻雜增彊瞭TiO2的Lewis痠性;負載WO3之後,位于3.1~1.7 nm之間孔隙的穩定性顯著增彊;NH3的吸附與活化分彆由TiO2-ZrO2載體和WO3完成;WO3中W元素彊大的電負性,促進瞭NH3的N—H鍵由共價鍵嚮離子鍵過渡,進而導緻瞭NH3的活化。脫硝活性結果顯示:噹WO3含量為9%(質量)時,催化劑脫硝活性最高,併在320~420℃的溫度窗口保持94%以上。(9%)WO3/TiO2-ZrO2具有更加穩定的孔隙結構(4.4~1.7 nm),錶麵Br?nsted痠中心數量增加,Lewis痠中心的彊度和痠量增加的幅度最大, NH3-SCR過程中的活性中間產物NH2的吸收峰更加明顯,這些特徵可能是其脫硝活性最好的原因。
채용공침정법제비료WO3/TiO2-ZrO2탈초최화제,병용고정상반응기진행활성평개,채용BET、XRD、TPD、안기흡부만반사FT-IR진행표정。결과현시,ZrO2참잡증강료TiO2적Lewis산성;부재WO3지후,위우3.1~1.7 nm지간공극적은정성현저증강;NH3적흡부여활화분별유TiO2-ZrO2재체화WO3완성;WO3중W원소강대적전부성,촉진료NH3적N—H건유공개건향리자건과도,진이도치료NH3적활화。탈초활성결과현시:당WO3함량위9%(질량)시,최화제탈초활성최고,병재320~420℃적온도창구보지94%이상。(9%)WO3/TiO2-ZrO2구유경가은정적공극결구(4.4~1.7 nm),표면Br?nsted산중심수량증가,Lewis산중심적강도화산량증가적폭도최대, NH3-SCR과정중적활성중간산물NH2적흡수봉경가명현,저사특정가능시기탈초활성최호적원인。
(x)WO3/TiO2-ZrO2 catalysts with different WO3 content were prepared by the impregnation method and the catalytic performance for the selective catalytic reduction of NOx with NH3(NH3-SCR) was investigated in a fixed-bed stainless steel reactor. The catalysts were characterized by BET, XRD, NH3-TPD andin situ DRIFTS analysis of NH3 adsorption, and revealed the change of the structural property and acidic capacity. The characterization results showed that WO3 was in a well-dispersed state and WO3addition enhanced the thermal stability of catalysts obviously. The adsorption and activation of NH3 were caused by TiO2-ZrO2and WO3, respectively. It was found that W displayed a huge electronegativity and prompted the transfer of the N—H bond of NH3 from covalent bond to ionic bond, which could incur theNH3activation. The results of catalytic activity indicated that the catalyst with 9%(mass) WO3 content exhibited 94% NO conversion within the wide temperature range of 320℃ to 420℃. (9%)WO3/TiO2-ZrO2possessed comparatively higher intensity of Lewis acidity and <br> larger amount of Br?nsted acidity as well as more stable pore structure (4.4—1.7 nm). Besides, the absorption peak of the active intermediate species NH2was more obvious. All these characters probably accounted for its better catalytic performance.