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): 2309036-0. doi: 10.3866/PKU.WHXB202309036
2. [2]
  Liangliang Song , Haoyan Liang , Shunqing Li , Bao Qiu , Zhaoping Liu . Challenges and strategies on high-manganese Li-rich layered oxide cathodes for ultrahigh-energy-density batteries. Acta Physico-Chimica Sinica, 2025, 41(8): 100085-0. doi: 10.1016/j.actphy.2025.100085
3. [3]
  .
  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): -.
4. [4]
  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
5. [5]
  Jingkun Yu , Xue Yong , Ang Cao , Siyu Lu . Bi-Layer Single Atom Catalysts Boosted Nitrate-to-Ammonia Electroreduction with High Activity and Selectivity. Acta Physico-Chimica Sinica, 2024, 40(6): 2307015-0. doi: 10.3866/PKU.WHXB202307015
6. [6]
  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): 2407005-0. doi: 10.3866/PKU.WHXB202407005
7. [7]
  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
8. [8]
  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
9. [9]
  Shijie Ren , Mingze Gao , Rui-Ting Gao , Lei Wang . Bimetallic Oxyhydroxide Cocatalyst Derived from CoFe MOF for Stable Solar Water Splitting. Acta Physico-Chimica Sinica, 2024, 40(7): 2307040-0. doi: 10.3866/PKU.WHXB202307040
10. [10]
  Jiahao Zeng , Hui Chao . 诱导程序性细胞死亡的金属抗肿瘤药物研究. University Chemistry, 2025, 40(6): 145-159. doi: 10.12461/PKU.DXHX202406019
11. [11]
  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
12. [12]
  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
13. [13]
  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
14. [14]
  Yu Wang , Haiyang Shi , Zihan Chen , Feng Chen , Ping Wang , Xuefei Wang . 具有富电子Pt^δ−壳层的空心AgPt@Pt核壳催化剂：提升光催化H₂O₂生成选择性与活性. Acta Physico-Chimica Sinica, 2025, 41(7): 100081-0. doi: 10.1016/j.actphy.2025.100081
15. [15]
  Ye Wang , Ruixiang Ge , Xiang Liu , Jing Li , Haohong Duan . An Anion Leaching Strategy towards Metal Oxyhydroxides Synthesis for Electrocatalytic Oxidation of Glycerol. Acta Physico-Chimica Sinica, 2024, 40(7): 2307019-0. doi: 10.3866/PKU.WHXB202307019
16. [16]
  Lijun Yue , Siya Liu , Peng Liu . 不同晶相纳米MnO₂的制备及其对生物乙醇选择性氧化催化性能的测试——一个科研转化的综合化学实验. University Chemistry, 2025, 40(8): 225-232. doi: 10.12461/PKU.DXHX202410005
17. [17]
  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): 2406012-0. doi: 10.3866/PKU.WHXB202406012
18. [18]
  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): 2404023-0. doi: 10.3866/PKU.WHXB202404023
19. [19]
  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
20. [20]
  Yan Kong , Wei Wei , Lekai Xu , Chen Chen . Electrochemical Synthesis of Organonitrogen Compounds from N-integrated CO₂ Reduction Reaction. Acta Physico-Chimica Sinica, 2024, 40(8): 2307049-0. doi: 10.3866/PKU.WHXB202307049

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(515)
HTML views(26)

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