Citation: CHEN Feng, HUANG Bi-Chun, YANG Ying-Xin, LIU Xiao-Qing, YU Cheng-Long. Synthesis, Characterization and NH₃-SCR Activity of MnSAPO-34 Molecular Sieves[J]. Acta Physico-Chimica Sinica, ;2015, 31(12): 2375-2385. doi: 10.3866/PKU.WHXB201510201 shu

Synthesis, Characterization and NH₃-SCR Activity of MnSAPO-34 Molecular Sieves

1.
1 School of Environment and Energy, South China University of Technology, Guangzhou 510006, P. R. China;
2.
2 Key Laboratory of the Ministry of Education for Pollution Control and Ecosystem Restoration in Industry Clusters, South China University of Technology, Guangzhou 510006, P. R. China

Corresponding author: HUANG Bi-Chun,
Received Date: 28 April 2015
Available Online: 19 October 2015
Fund Project: 国家自然科学基金(51478191) (51478191)广东省省级科技计划项目(2014A020216003)资助 (2014A020216003)

A series of MnSAPO-34 molecular sieves were synthesized by a hydrothermal method for selective catalytic reduction (SCR) of NO with NH₃ and characterized using X-ray photoelectron spectroscopy (XPS), temperature-programmed reduction (TPR), and temperature-programmed desorption (TPD). Three factors were studied, including Mn-loading, calcination temperature, and synthesis time. The MnSAPO-34, which was synthesized in 6 h and calcined at 550 ℃ with the Mn-loading (n_(MnO)/n_(P₂O₅)= 0.1), exhibits the highest activity among all the samples, with NO_x conversion of almost 100% and N₂ selectivity higher than 80%. The results show that the porous and crystalline structures of MnSAPO-34 are greatly affected by addition of manganese, and excessive Mn-loading could result in lower crystallinity and the generation of nonframework manganese oxides. Meanwhile, a decrease in specific surface area and pore volume are observed in MnSAPO-34 with higher Mn-loading; however, the opposite characteristics are observed with a decreasing calcination temperature and shorter synthesis time. Manganese species of high oxidation state, mostly Mn⁴⁺, are shown to be on the catalysts surface after high temperature calcination, and the increase ratio of Mn³⁺ could help to improve the catalytic activity. Under proper synthesis conditions, the incorporation of manganese could improve the adsorption of nitric oxide and ammonia, and the interaction between the strongly adsorbed NO and strongly adsorbed NH₃ might be the reason for the enhancement in their catalytic efficiency.
- Selective catalytic reduction,
- Nitrogen oxide,
- Manganese,
- SAPO-34 molecular sieve,
- X-ray photoelectron spectroscopy,
- Temperature-programmed reduction
1. [1]
  (1) Qi, G. S.; Yang, R. T. Appl. Catal. B-Environ. 2003, 44, 217. doi: 10.1016/S0926-3373(03)00100-0
2. [2]
  (2) Fang, C.; Zhang, D. S.; Cai, S. X.; Zhang, L.; Huang, L.; Li, H. R.; Maitarad, P.; Shi, L. Y.; Gao, R. H.; Zhang, J. P. Nanoscale 2013, 5, 9199. doi: 10.1039/c3nr02631k
3. [3]
  (3) Wang, L. S.; Huang, B. C.; Su, Y. X.; Zhou, G. Y.; Wang, K. L.; Luo, H. C.; Ye, D. Q. Chem. Eng. J. 2012, 192, 232. doi: 10.1016/j.cej.2012.04.012
4. [4]
  (4) Su, Y. X.; Fan, B. X.; Wang, L. S.; Liu, Y. F.; Huang, B. C.; Fu, M. L.; Chen, L. M.; Ye, D. Q. Catal. Today 2013, 201, 115. doi: 10.1016/j.cattod.2012.04.063
5. [5]
  (5) Huang, P.; Pan, S. W.; Huang, B. C.; Cheng, H.; Ye, D. Q.; Wu, J. L.; Fu, M. L.; Lu, S. L. Acta Phys. -Chim. Sin. 2013, 29, 176. [黄萍, 盘思伟, 黄碧纯, 程华, 叶代启, 吴军良, 付名利, 卢圣良. 物理化学学报, 2013, 29, 176.] doi: 10.3866/PKU.WHXB201210094
6. [6]
  (6) Yang, C.; Liu, X. Q.; Huang, B. C.; Wu, Y. M. Acta Phys. -Chim. Sin. 2014, 30, 1895. [杨超, 刘小青, 黄碧纯, 吴友明. 物理化学学报, 2014, 30, 1895.] doi: 10.3866/PKU.WHXB201407162
7. [7]
  (7) Yu, C. L.; Huang, B. C.; Yang, Y. X. Journal of South China University of Technology (Natural Science Edition) 2015, 3, 143. [喻成龙, 黄碧纯, 杨颖欣. 华南理工大学学报(自然科学版), 2015, 3, 143.]
8. [8]
  (8) Xue, J. J.; Wang, X. Q.; Qi, G. S.; Wang, J.; Shen, M. Q.; Li, W. J. Catal. 2013, 297, 56. doi: 10.1016/j.jcat.2012.09.020
9. [9]
  (9) Wang, J.; Yu, T.; Wang, X. Q.; Qi, G. S.; Xue, J. J.; Shen, M. Q.; Li, W. Appl. Catal. B-Environ. 2012, 127, 137. doi: 10.1016/j.apcatb.2012.08.016
10. [10]
  (10) Ye, Q.; Wang, L. F.; Yang, R. T. Appl. Catal. A-Gen. 2012, 427-428, 24.
11. [11]
  (11) Martí nez-Franco, R.; Moliner, M.; Franch, C.; Kustov, A.; Corma, A. Appl. Catal. B-Environ. 2012, 127, 273. doi: 10.1016/j.apcatb.2012.08.034
12. [12]
  (12) Martí nez-Franco, R.; Moliner, M.; Concepcion, P.; Thogersen, J. R.; Corma, A. J. Catal. 2014, 314, 73. doi: 10.1016/j.jcat.2014.03.018
13. [13]
  (13) Deka, U.; Lezcano-Gonzalez, I.; Warrender, S. J.; Picone, A. L.; Wright, P. A.; Weckhuysen, B. M.; Beale, A. M. Microporous Mesoporous Mat. 2013, 166, 144. doi: 10.1016/j.micromeso.2012.04.056
14. [14]
  (14) Wei, Y. X.; He, Y. L.; Zhang, D. Z.; Xu, L.; Meng, S. H.; Liu, Z. M.; Su, B. L. Microporous Mesoporous Mat. 2006, 90, 188. doi: 10.1016/j.micromeso.2005.10.042
15. [15]
  (15) Tuš ar, N. N.; Mali, G.; Arć on, I.; Kauč ič , V.; Ghanbari-Siahkali, A.; Dwyer, J. Microporous Mesoporous Mat. 2002, 55, 203. doi: 10.1016/S1387-1811(02)00404-3
16. [16]
  (16) Rajić , N.; Stojaković , D.; Hoç evar, S.; Kauč ič , V. Zeolites 1993, 13, 384. doi: 10.1016/0144-2449(93)90154-U
17. [17]
  (17) Gu, J. F.; Agula, B.; Jia, M. L.; Liu, Y. P.; Zhaorigetu, B.; Yuan, Z. Y. Chin. J. Catal. 2010, 31, 322. [顾建峰, 阿古拉, 贾美林, 刘玉萍, 照日格图, 袁忠勇. 催化学报, 2010, 31, 322.]
18. [18]
  (18) Zhang, R. Z.; Zhao, L. F. Impurity Atoms of Phosphorus Aluminum Molecular Sieve and Its Application; Chemical Industry Press: Beijing, 2009; pp 56-57. [张瑞珍, 赵亮富. 杂原子磷铝分子筛及应用. 北京: 化学工业出版社, 2009: 56-57.]
19. [19]
  (19) Qi, G. S.; Yang, R. T. J. Phys. Chem. B 2004, 108, 15738. doi: 10.1021/jp048431h
20. [20]
  (20) Kapteijn, F.; Singoredjo, L.; Andreini, A.; Moulijn, J. A. Appl. Catal. B-Environ. 1994, 3, 173. doi: 10.1016/0926-3373(93)E0034-9
21. [21]
  (21) Tian, P.; Liu, Z. M.; Wu, Z. B.; Xu, L.; He, Y. L. Catal. Today 2004, 93-95, 735.
22. [22]
  (22) Thomas, J. M.; Greaves, G. N. Science 1994, 265, 1675.
23. [23]
  (23) Ramesh, K.; Chen, L. W.; Chen, F. X.; Liu, Y.; Wang, Z.; Han, Y. F. Catal. Today 2008, 131, 477. doi: 10.1016/j.cattod.2007.10.061
24. [24]
  (24) Wang, L. C.; Liu, Q.; Huang, X. S.; Liu, Y. M.; Cao, Y.; Fan, K. N. Appl. Catal. B-Environ. 2009, 88, 204. doi: 10.1016/j.apcatb.2008.09.031
25. [25]
  (25) Ristić , A.; Logar, N. Z.; Henninger, S. K.; Kauč ič , V. Adv. Funct. Mater. 2012, 22, 1952. doi: 10.1002/adfm.201102734
26. [26]
  (26) Ponce, S.; Peň a, M. A.; Fierro, J. L. G. Appl. Catal. B-Environ. 2000, 24, 193. doi: 10.1016/S0926-3373(99)00111-3
27. [27]
  (27) Kang, M.; Park, E. D.; Kim, J. M.; Yie, J. E. Appl. Catal. A-Gen. 2007, 327, 261. doi: 10.1016/j.apcata.2007.05.024
28. [28]
  (28) Akolekar, D. B.; Bhargava, S. K. Appl. Catal. A-Gen. 2001, 207, 355. doi: 10.1016/S0926-860X(00)00669-4
29. [29]
  (29) Lu, X.; Song, C.; Chang, C.; Teng, Y.; Tong, Z.; Tang, X. Ind. Eng. Chem. Res. 2014, 53, 11601. doi: 10.1021/ie5016969
30. [30]
  (30) Park, E.; Kim, M.; Jung, H.; Chin, S.; Jurng, J. ACS Catal. 2013, 3, 1518. doi: 10.1021/cs3007846
31. [31]
  (31) Vieira, A.; Tovar, M. A.; Pfaff, C.; Betancourt, P.; Méndez, B.; López, C. M.; Machado, F. J.; Goldwasser, J.; de Agudelo, M. M. R.; Houalla, M. J. Mol. Catal. A-Chem. 1999, 144, 101. doi: 10.1016/S1381-1169(98)00338-0
32. [32]
  (32) Wu, Z. B.; Jiang, B. Q.; Liu, Y.; Wang, H. Q.; Jin, R. B. Environ. Sci. Technol. 2007, 41, 5812. doi: 10.1021/es0700350
33. [33]
  (33) Liu, F. D.; He, H. Catal. Today 2010, 153, 70. doi: 10.1016/j.cattod.2010.02.043
34. [34]
  (34) Guan, B.; Lin, H.; Zhu, L.; Huang, Z. J. Phys. Chem. C 2011, 115, 12850. doi: 10.1021/jp112283g
35. [35]
  (35) Shu, Y.; Sun, H.; Quan, X.; Chen, S. J. Phys. Chem. C 2012, 116, 25319. doi: 10.1021/jp307038q
36. [36]
  (36) Yu, C. L.; Wang, L. S.; Huang, B. C. Aerosol Air Qual. Res. 2015, 15, 1017.
37. [37]
  (37) Vishwanathan, V.; Jun, K. W.; Kim, J. W.; Roh, H. S. Appl. Catal. A-Gen. 2004, 276, 251.
38. [38]
  (38) Jin, R. B.; Liu. Y.; Wu, Z. B.; Wang, H. Q.; Gu, T. T. Catal. Today 2010, 153, 84. doi: 10.1016/j.cattod.2010.01.039
39. [39]
  (39) Fang, C.; Zhang, D. S.; Shi, L. Y.; Gao, R. H.; Li, H. R.; Ye, L. P.; Zhang, J. P. Catal. Sci. Technol. 2013, 3, 803. doi: 10.1039/C2CY20670F
1. [1]
  Chongjing Liu , Yujian Xia , Pengjun Zhang , Shiqiang Wei , Dengfeng Cao , Beibei Sheng , Yongheng Chu , Shuangming Chen , Li Song , Xiaosong Liu . Understanding Solid-Gas and Solid-Liquid Interfaces through Near Ambient Pressure X-Ray Photoelectron Spectroscopy. Acta Physico-Chimica Sinica, 2025, 41(2): 100013-. doi: 10.3866/PKU.WHXB202309036
2. [2]
  .
  CCS Chemistry | 超分子活化底物为自由基促进高效选择性光催化氧化
  . CCS Chemistry, 2025, 7(10.31635/ccschem.025.202405229): -.
3. [3]
  Yufang GAO , Nan HOU , Yaning LIANG , Ning LI , Yanting ZHANG , Zelong LI , Xiaofeng LI . Nano-thin layer MCM-22 zeolite: Synthesis and catalytic properties of trimethylbenzene isomerization reaction. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1079-1087. doi: 10.11862/CJIC.20240036
4. [4]
  Xiaofeng Zhu , Bingbing Xiao , Jiaxin Su , Shuai Wang , Qingran Zhang , Jun Wang . Transition Metal Oxides/Chalcogenides for Electrochemical Oxygen Reduction into Hydrogen Peroxides. Acta Physico-Chimica Sinica, 2024, 40(12): 2407005-. doi: 10.3866/PKU.WHXB202407005
5. [5]
  Peng YUE , Liyao SHI , Jinglei CUI , Huirong ZHANG , Yanxia GUO . Effects of Ce and Mn promoters on the selective oxidation of ammonia over V₂O₅/TiO₂ catalyst. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 293-307. doi: 10.11862/CJIC.20240210
6. [6]
  Junjie Zhang , Yue Wang , Qiuhan Wu , Ruquan Shen , Han Liu , Xinhua Duan . Preparation and Selective Separation of Lightweight Magnetic Molecularly Imprinted Polymers for Trace Tetracycline Detection in Milk. University Chemistry, 2024, 39(5): 251-257. doi: 10.3866/PKU.DXHX202311084
7. [7]
  Yingchun ZHANG , Yiwei SHI , Ruijie YANG , Xin WANG , Zhiguo SONG , Min WANG . Dual ligands manganese complexes based on benzene sulfonic acid and 2, 2′-bipyridine: Structure and catalytic properties and mechanism in Mannich reaction. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1501-1510. doi: 10.11862/CJIC.20240078
8. [8]
  Xilin Zhao , Xingyu Tu , Zongxuan Li , Rui Dong , Bo Jiang , Zhiwei Miao . Research Progress in Enantioselective Synthesis of Axial Chiral Compounds. University Chemistry, 2024, 39(11): 158-173. doi: 10.12461/PKU.DXHX202403106
9. [9]
  Ping ZHANG , Chenchen ZHAO , Xiaoyun CUI , Bing XIE , Yihan LIU , Haiyu LIN , Jiale ZHANG , Yu'nan CHEN . Preparation and adsorption-photocatalytic performance of ZnAl@layered double oxides. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1965-1974. doi: 10.11862/CJIC.20240014
10. [10]
  Xin Han , Zhihao Cheng , Jinfeng Zhang , Jie Liu , Cheng Zhong , Wenbin Hu . Design of Amorphous High-Entropy FeCoCrMnBS (Oxy) Hydroxides for Boosting Oxygen Evolution Reaction. Acta Physico-Chimica Sinica, 2025, 41(4): 100033-. doi: 10.3866/PKU.WHXB202404023
11. [11]
  Zhuo WANG , Junshan ZHANG , Shaoyan YANG , Lingyan ZHOU , Yedi LI , Yuanpei LAN . Preparation and photocatalytic performance of CeO₂-reduced graphene oxide by thermal decomposition. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1708-1718. doi: 10.11862/CJIC.20240067
12. [12]
  Pei Li , Yuenan Zheng , Zhankai Liu , An-Hui Lu . Boron-Containing MFI Zeolite: Microstructure Control and Its Performance of Propane Oxidative Dehydrogenation. Acta Physico-Chimica Sinica, 2025, 41(4): 100034-. doi: 10.3866/PKU.WHXB202406012
13. [13]
  Jiali CHEN , Guoxiang ZHAO , Yayu YAN , Wanting XIA , Qiaohong LI , Jian ZHANG . Machine learning exploring the adsorption of electronic gases on zeolite molecular sieves. Chinese Journal of Inorganic Chemistry, 2025, 41(1): 155-164. doi: 10.11862/CJIC.20240408
14. [14]
  Qianwen Han , Tenglong Zhu , Qiuqiu Lü , Mahong Yu , Qin Zhong . 氢电极支撑可逆固体氧化物电池性能及电化学不对称性优化. Acta Physico-Chimica Sinica, 2025, 41(1): 2309037-. doi: 10.3866/PKU.WHXB202309037
15. [15]
  Shihui Shi , Haoyu Li , Shaojie Han , Yifan Yao , Siqi Liu . Regioselectively Synthesis of Halogenated Arenes via Self-Assembly and Synergistic Catalysis Strategy. University Chemistry, 2024, 39(5): 336-344. doi: 10.3866/PKU.DXHX202312002
16. [16]
  Bing WEI , Jianfan ZHANG , Zhe CHEN . Research progress in fine tuning of bimetallic nanocatalysts for electrocatalytic carbon dioxide reduction. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 425-439. doi: 10.11862/CJIC.20240201
17. [17]
  Lina Guo , Ruizhe Li , Chuang Sun , Xiaoli Luo , Yiqiu Shi , Hong Yuan , Shuxin Ouyang , Tierui Zhang . 层状双金属氢氧化物的层间阴离子对衍生的Ni-Al₂O₃催化剂光热催化CO₂甲烷化反应的影响. Acta Physico-Chimica Sinica, 2025, 41(1): 2309002-. doi: 10.3866/PKU.WHXB202309002
18. [18]
  Yunting Shang , Yue Dai , Jianxin Zhang , Nan Zhu , Yan Su . Something about RGO (Reduced Graphene Oxide). University Chemistry, 2024, 39(9): 273-278. doi: 10.3866/PKU.DXHX202306050
19. [19]
  Junli Liu . Practice and Exploration of Research-Oriented Classroom Teaching in the Integration of Science and Education: a Case Study on the Synthesis of Sub-Nanometer Metal Oxide Materials and Their Application in Battery Energy Storage. University Chemistry, 2024, 39(10): 249-254. doi: 10.12461/PKU.DXHX202404023
20. [20]
  Yaping ZHANG , Tongchen WU , Yun ZHENG , Bizhou LIN . Z-scheme heterojunction β-Bi₂O₃ pillared CoAl layered double hydroxide nanohybrid: Fabrication and photocatalytic degradation property. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 531-539. doi: 10.11862/CJIC.20240256

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(441)
HTML views(21)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Synthesis, Characterization and NH3-SCR Activity of MnSAPO-34 Molecular Sieves

Metrics

通讯作者: 陈斌, bchen63@163.com

Synthesis, Characterization and NH₃-SCR Activity of MnSAPO-34 Molecular Sieves