| 22 | 0 | 72 |
| 下载次数 | 被引频次 | 阅读次数 |
为了提高Cu-SSZ-39分子筛在NH3选择性催化还原(NH3-SCR)反应中的催化性能，通过离子交换法制备了Cu-Sm-SSZ-39分子筛，并使用X射线衍射、NH3程序升温脱附等表征手段研究了掺杂Sm对Cu-SSZ-39分子筛的性能影响。结果表明：在400～600℃的高温范围内，Cu-Sm-SSZ-39的NO转化率始终维持在60%以上，其NO转化率比相同温度下的Cu-SSZ-39的NO转化率高3%～9%;Cu-Sm-SSZ-39可以在183～513℃内保持80%以上的NO转化率，与Cu-SSZ-39相比这一范围增大了7.3%；经过水热老化后Cu-Sm-SSZ-39的比表面积降低了0.5%～1.8%，比表面积的损失量要小于Cu-SSZ-39的损失量；Sm3+还可以在水热老化过程中减少分子筛中的酸性位点和活性Cu物种的损失，减小因Cu2+迁移现象而生成的CuOx团簇的含量。
Abstract：In order to improve the catalytic performance of Cu-SSZ-39 zeolite in the NH3 selective catalytic reduction(NH3-SCR) reaction, Cu-Sm-SSZ-39 molecular sieves was prepared by ion exchange method. Characterization methods, such as X-ray diffraction and NH3 temperature-programmed desorption, were used to study the effect of Sm doping on the performance of Cu-SSZ-39 zeolite. The results show that within the high temperature range of 400—600 ℃, the NO conversion rate of Cu-Sm-SSZ-39 remains above 60%, and its NO conversion rate is3%—9% higher than that of Cu-SSZ-39 at the same temperature. Cu-Sm-SSZ-39 can maintain a NO conversion rate of over 80% within the temperature range of 183—513 ℃, and this range is increased by 7.3% compared with Cu-SSZ-39. Moreover, after hydrothermal aging, the specific surface area of Cu-Sm-SSZ-39 is reduced by only 0.5% —1.8%, and the loss of specific surface area is less than that of Cu-SSZ-39. In addition,Sm3+can also reduce the loss of acid sites and active Cu species in the zeolite during hydrothermal aging, and reduce the content of CuO_xclusters generated due to Cu2+migration.
[1]SHAN W P,SONG H.Catalysts for the selective catalytic reduction of NOxwith NH3at low temperature[J].Catalysis Science&Technology,2015,5(9):4280-4288.
[2]SONG Z X,ZHANG Q L,NING P,et al.Effect of copper precursors on the catalytic activity of Cu/ZSM-5 catalysts for selective catalytic reduction of NO by NH3[J].Research on Chemical Intermediates,2016,42(10):7429-7445.
[3]GUO A Q,LIU H B,LI Y T,et al.Recent progress in novel zeolite catalysts for selective catalytic reduction of nitrogen oxides[J].Catalysis Today,2023,422:114212.
[4]MART魱N N,VENNESTRØM P N R,THØGERSEN J R,et al.Iron-containing SSZ-39 (AEI) zeolite:An active and stable high-temperature NH3-SCR catalyst[J].Chem Cat Chem,2017,9(10):1754-17577.
[5]SHAN Y L,DU J P,ZHANG Y,et al.Selective catalytic reduction of NOxwith NH3:Opportunities and challenges of Cubased small-pore zeolites[J].National Science Review,2021,8(10):nwab010.
[6]ZHANG S T,PANG L,CHEN Z,et al.Cu/SSZ-13 and Cu/SAPO-34 catalysts for de NOxin diesel exhaust:Current status,challenges,and future perspectives[J].Applied Catalysis A:General,2020,607:117855.
[7]LI X Y,ZHAO H W,HUANG Y T,et al.Boosting the lowtemperature activity of Cu-SSZ-13 for NH3-SCR by mixing Mn Ce Ti Ox:The effect of nitrates on Cu redox cycle[J].Journal of Environmental Chemical Engineering,2022,10 (6):109016.
[8]UCHISAWA J,OBUCHI A,YAMAMOTO A,et al.Effect of water vapor on the accelerated deterioration treatment of CuSSZ-13 as catalysts for selective catalytic reduction[J].Industrial&Engineering Chemistry Research,2021,60 (43):15454-15463.
[9]XI Y Z,SU C S,OTTINGER N A,et al.Effects of hydrothermal aging on the sulfur poisoning of a Cu-SSZ-13 SCR catalyst[J].Applied Catalysis B:Environmental,2021,284:119749.
[10]MA Y,CHENG S Q,WU X D,et al.Improved hydrothermal durability of Cu-SSZ-13 NH3-SCR catalyst by surface Al modification:Affinity and passivation[J].Journal of Catalysis,2022,405:199-211.
[11]TIAN Z G,LI X,CAO Y X,et al.Photoluminescence properties of Eu2+-doped microporous zeolite SSZ-39 with color tunable emission[J].Journal of Luminescence,2019,211:62-68.
[12]MOLINER M,FRANCH C,PALOMARES E,et al.Cu-SSZ-39,an active and hydrothermally stable catalyst for the selective catalytic reduction of NOx[J].Chemical Communications,2012,48(66):8264-8266.
[13]SHAN Y L,SHAN W P,SHI X Y,et al.A comparative study of the activity and hydrothermal stability of Al-rich Cu-SSZ-39 and Cu-SSZ-13[J].Applied Catalysis B:Environmental,2020,264:118511.
[14]ZHAO Z C,YU R,SHI C,et al.Rare-earth ion exchanged Cu-SSZ-13 zeolite from organotemplate-free synthesis with enhanced hydrothermal stability in NH3-SCR of NOx[J].Catalysis Science&Technology,2019,9(1):241-251.
[15]WANG Y,LI G G,ZHANG S Q,et al.Promoting effect of Ce and Mn addition on Cu-SSZ-39 zeolites for NH3-SCR reaction:Activity,hydrothermal stability,and mechanism study[J].Chemical Engineering Journal,2020,393:124782.
[16]LIN Q J,XU S H,ZHAO H Y,et al.Highlights on key roles of Y on the hydrothermal stability at 900℃of Cu/SSZ-39 for NH3-SCR[J].ACS Catalysis,2022,12(22):14026-14039.
[17]WANG Y J,SHI X Y,SHAN Y L,et al.Hydrothermal stability enhancement of Al-rich Cu-SSZ-13 for NH3selective catalytic reduction reaction by ion exchange with cerium and samarium[J].Industrial&Engineering Chemistry Research,2020,59(14):6416-6423.
[18]CHEN M Y,LI J Y,XUE W J,et al.Unveiling secondaryion-promoted catalytic properties of Cu-SSZ-13 zeolites for selective catalytic reduction of NOx[J].Journal of the American Chemical Society,2022,144(28):12816-12824.
[19]YU R,KONG H Y,ZHAO Z C,et al.Rare-earth yttrium exchanged Cu-SSZ-39 zeolite with superior hydrothermal stability and SO2-tolerance in NH3-SCR of NOx[J].Chem Cat Chem,2022,14(10):e202200228.
[20]ZHU N,SHAN W P,SHAN Y L,et al.Effects of alkali and alkaline earth metals on Cu-SSZ-39 catalyst for the selective catalytic reduction of NOxwith NH3[J].Chemical Engineering Journal,2020,388:124250.
[21]SUN G,YU R,XU L L,et al.Enhanced hydrothermal stability and SO2-tolerance of Cu-Fe modified AEI zeolite catalysts in NH3-SCR of NOx[J].Catalysis Science&Technology,2022,12(12):3898-3911.
基本信息:
中图分类号:TQ426;X701
引用信息:
[1]李渊,杨东旭,曹依凡.稀土Sm掺杂对Cu-SSZ-39分子筛的结构调控及NH_3-SCR性能增强机理[J].天津工业大学学报,2026,45(01):31-37.
基金信息:
国家自然科学基金项目（91745116）
2026-02-25
2026-02-25