Citation: Zhen Chen, Ce Bian, Chi Fan, Tao Li. The role of Si coordination structures in the catalytic properties and durability of Cu-SAPO-34 as NH₃-SCR catalyst for NO_x reduction[J]. Chinese Chemical Letters, ;2022, 33(2): 893-897. doi: 10.1016/j.cclet.2021.06.071 shu

The role of Si coordination structures in the catalytic properties and durability of Cu-SAPO-34 as NH₃-SCR catalyst for NO_x reduction

Zhen Chen ¹ ,
Ce Bian ¹ ,
Chi Fan ,
Tao Li ^*,

Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, China

taoli@hust.edu.cn

Received Date: 19 January 2021
Revised Date: 14 May 2021
Accepted Date: 25 June 2021
Available Online: 2 July 2021

Figures(4)

Si coordination structures have been proven to greatly influence the ammonia-selective catalytic reduction (NH₃-SCR) catalytic properties and the hydrothermal stability of Cu-based silicoaluminophosphate-form catalysts. However, the role of various Si coordination structures in the NH₃-SCR reaction over Cu-SAPO-34 catalyst remains unknown. Herein, a batch of Cu-SAPO-34 samples with various Si contents was synthesized via a one-pot method to study the role of Si coordination structures in the NH₃-SCR catalytic properties and hydrothermal stability. Cu/34–2 with the highest proportion of Si(xOAl) (x = 1~3) structures exhibits remarkable durability with 90% NO reduction efficiency within 200~450 ℃ even after a hydrothermal aging treatment at 850 ℃. In contrast, Cu/34–1 and Cu/34–4 with the highest proportions of Si(4OAl) and Si(0OAl) structures, respectively, are significantly deactivated by the same hydrothermal treatment. To better understand this phenomenon, the relationship between the Si coordination structures and SCR performance is established using characterization techniques and kinetics measurements. Results reveal that a high content of Si(4OAl) and Si(0OAl) is detrimental to the hydrothermal stability of Cu-SAPO-34 catalyst. However, Si(xOAl) (x = 1~3) structures are conducive to the stabilization of isolated Cu²⁺, thus enhancing the stability to severe hydrothermal treatment.
- NO_x,
- NH₃-SCR,
- Cu-SAPO-34,
- Si coordination structure,
- Hydrothermal stability
1. [1]
  Y. Tan, P. Henderick, S. Yoon, et al., Environ. Sci. Technol.53 (2019) 5504–5511. doi: 10.1021/acs.est.8b07048
2. [2]
  J. Du, X. Shi, Y. Shan, et al., Environ. Sci. Technol. 54 (2020) 7870–7878. doi: 10.1021/acs.est.0c01743
3. [3]
  A.M. Beale, F. Gao, I. Lezcano-Gonzalez, C.H.F. Peden, J. Szanyi, Chem. Soc. Rev. 44 (2015) 7371–7405. doi: 10.1039/C5CS00108K
4. [4]
  S. Zhang, L. Pang, Z. Chen, et al., Appl. Catal. A607 (2020) 117855. doi: 10.1016/j.apcata.2020.117855
5. [5]
  L. Sun, M. Yang, Y. Cao, et al., Chin. J. Catal. 41 (2020) 1410–1420. doi: 10.1016/S1872-2067(20)63583-5
6. [6]
  D. Wang, Y. Jangjou, Y. Liu, et al., Appl. Catal. B165 (2015) 438–445. doi: 10.1016/j.apcatb.2014.10.020
7. [7]
  L. Wang, J. Wan, Y. Zhao, N. Yang, D. Wang, J. Am. Chem. Soc. 141 (2019) 2238–2241. doi: 10.1021/jacs.8b13528
8. [8]
  F. You, J. Wan, J. Qi, et al., Angew. Chem., Int. Ed. 132 (2020) 731–734. doi: 10.1002/ange.201912069
9. [9]
  H. Wang, J. Qi, N. Yang, et al., Angew. Chem. Int. Ed. 59 (2020) 19691–19695. doi: 10.1002/anie.202007077
10. [10]
  H. Wang, D. Mao, J. Qi, et al., Adv. Funct. Mater. 29 (2019) 1806588. doi: 10.1002/adfm.201806588
11. [11]
  Y. Wei, J. Wan, N. Yang, et al. Natl. Sci. Rev. 7 (2020) 1638–1646. doi: 10.1093/nsr/nwaa059
12. [12]
  Z. Chen, C. Fan, L. Pang, et al., Appl. Surf. Sci. 448 (2018) 671–680. doi: 10.1016/j.apsusc.2018.04.076
13. [13]
  D. Zhang, R.T. Yang, Appl. Catal. A543 (2017) 247–256. doi: 10.1016/j.apcata.2017.06.021
14. [14]
  C. Niu, X. Shi, K. Liu, et al., Catal. Commun. 81 (2016) 20–23. doi: 10.1016/j.catcom.2016.04.007
15. [15]
  L. Wang, J.R. Gaudet, W. Li, D. Weng, J. Catal. 306 (2013) 68–77. doi: 10.1016/j.jcat.2013.06.010
16. [16]
  X. Liu, X. Wu, D. Weng, Z. Si, R. Ran, Catal. Today281 (2017) 596–604. doi: 10.1016/j.cattod.2016.05.021
17. [17]
  L. Wang, W. Li, S.J. Schmieg, D. Weng, J. Catal. 324 (2015) 98–106. doi: 10.1016/j.jcat.2015.01.011
18. [18]
  R. Martínez-Franco, M. Moliner, C. Franch, A. Kustov, A. Corma, Appl. Catal. B127 (2012) 273–280. doi: 10.1016/j.apcatb.2012.08.034
19. [19]
  J. Wang, T. Yu, X. Wang, et al., Appl. Catal. B127 (2012) 137–147. doi: 10.1016/j.apcatb.2012.08.016
20. [20]
  R. Martínez-Franco, M. Moliner, A. Corma, J. Catal. 319 (2014) 36–43. doi: 10.1016/j.jcat.2014.08.005
21. [21]
  Z. Chen, C. Fan, L. Pang, et al., Chem. Eng. J. 348 (2018) 608–617. doi: 10.1016/j.cej.2018.05.033
22. [22]
  W. Shen, X. Li, Y. Wei, et al., Micropor. Mesopor. Mater. 158 (2012) 19–25. doi: 10.1016/j.micromeso.2012.03.013
23. [23]
  M. Xu, J. Wang, T. Yu, J. Wang, M. Shen, Appl. Catal. B220 (2018) 161–170. doi: 10.1016/j.apcatb.2017.08.031
24. [24]
  R. Martínez-Franco, M. Moliner, P. Concepcion, J.R. Thogersen, A. Corma, J. Catal. 314 (2014) 73–82. doi: 10.1016/j.jcat.2014.03.018
25. [25]
  D. Fan, J. Wang, T. Yu, et al., Chem. Eng. Sci. 176 (2018) 285–293. doi: 10.1016/j.ces.2017.10.032
26. [26]
  R. Li, P. Wang, S. Ma, et al., Chem. Eng. J. 379 (2020) 122376. doi: 10.1016/j.cej.2019.122376
27. [27]
  Y. Wan, G. Yang, J. Xiang, et al., Dalton Trans. 49 (2020) 764–773. doi: 10.1039/c9dt03848e
28. [28]
  T. Yu, D. Fan, T. Hao, et al., Chem. Eng. J. 243 (2014) 159–168. doi: 10.1016/j.cej.2014.01.008
29. [29]
  X. Shen, Y. Du, J. Ding, et al., ChemCatChem12 (2020) 4904–4910. doi: 10.1002/cctc.202000794
30. [30]
  G. Pétaud, F. Gaillard, M. Tayakout, S. Gil, A. Giroir-Fendler, ChemCatChem12 (2020) 2807–2822. doi: 10.1002/cctc.201902036
31. [31]
  Y. Ma, X. Wu, L. Liu, et al., Appl. Catal. B278 (2020) 119306. doi: 10.1016/j.apcatb.2020.119306
32. [32]
  J. Cheng, S. Han, Q. Ye, et al., Res. Chem. Intermed. 45 (2019) 2023–2044. doi: 10.1007/s11164-018-03712-0
33. [33]
  M. Urrutxua, B. Pereda-Ayo, U. De-La-Torre, J.R. González-Velasco, ACS Omega 4 (2019) 14699–14713. doi: 10.1021/acsomega.9b01118
34. [34]
  U. Deka, I. Lezcano-Gonzalez, S.J. Warrender, et al., Microporous Mesoporous Mater. 166 (2013) 144–152. doi: 10.1016/j.micromeso.2012.04.056
35. [35]
  C. Wang, W. Yan, Z. Wang, et al., Catal. Today 355 (2020) 482–492. doi: 10.1016/j.cattod.2019.06.074
36. [36]
  S. Valange, Z. Gabelica, M. Abdellaoui, J. Clacens, J. Barrault, Microporous Mesoporous Mater. 30 (1999) 177–185. doi: 10.1016/S1387-1811(99)00031-1
37. [37]
  L. Xie, F. Liu, L. Ren, et al., Environ. Sci. Technol. 48 (2013) 566–572.
38. [38]
  Y. Ma, X. Wu, S. Cheng, et al., Appl. Catal. A602 (2020) 117650. doi: 10.1016/j.apcata.2020.117650
39. [39]
  G. Pétaud, S. Gil, A. Giroir-Fendler, M. Tayakout-Fayolle, Ind. Eng. Chem. Res. 59 (2020) 15848–15864. doi: 10.1021/acs.iecr.0c02270
40. [40]
  T. Yu, J. Wang, M. Shen, W. Li, Catal. Sci. Technol. 3 (2013) 3234–3241. doi: 10.1039/c3cy00453h
41. [41]
  D. Wang, L. Zhang, J. Li, K. Kamasamudram, W.S. Epling, Catal. Today231 (2014) 64–74. doi: 10.1016/j.cattod.2013.11.040
1. [1]
  Feibin Wei , Yongfang Rao , Yu Huang , Wei Wang , Hui Mei . The new challenges for the development of NH₃-SCR catalysts under new situation of energy transition in power generation industry. Chinese Chemical Letters, 2024, 35(6): 108931-. doi: 10.1016/j.cclet.2023.108931
2. [2]
  Lijun Yan , Shiqi Chen , Penglu Wang , Xiangyu Liu , Lupeng Han , Tingting Yan , Yuejin Li , Dengsong Zhang . Hydrothermally stable metal oxide-zeolite composite catalysts for low-temperature NO_x reduction with improved N₂ selectivity. Chinese Chemical Letters, 2024, 35(6): 109132-. doi: 10.1016/j.cclet.2023.109132
3. [3]
  Linhui Liu , Wuwan Xiong , Mingli Fu , Junliang Wu , Zhenguo Li , Daiqi Ye , Peirong Chen . Efficient NO_x abatement by passive adsorption over a Pd-SAPO-34 catalyst prepared by solid-state ion exchange. Chinese Chemical Letters, 2024, 35(4): 108870-. doi: 10.1016/j.cclet.2023.108870
4. [4]
  Zhengzhong Zhu , Shaojun Hu , Zhi Liu , Lipeng Zhou , Chongbin Tian , Qingfu Sun . A cationic radical lanthanide organic tetrahedron with remarkable coordination enhanced radical stability. Chinese Chemical Letters, 2025, 36(2): 109641-. doi: 10.1016/j.cclet.2024.109641
5. [5]
  Haiming Wu , Gaya N. Andrew , Rajini Anumula , Zhixun Luo . Corrigendum to 'How ligand coordination and superatomic-states accommodate the structure and property of a metal cluster: Cu₄ (dppy)₄ Cl₂ vs. Cu₂₁ (dppy)₁₀ with altered photoluminescence' [Chin. Chem. Lett. 35 (2024) 108340]. Chinese Chemical Letters, 2024, 35(12): 109912-. doi: 10.1016/j.cclet.2024.109912
6. [6]
  Yuan ZHU , Xiaoda ZHANG , Shasha WANG , Peng WEI , Tao YI . Conditionally restricted fluorescent probe for Fe³⁺ and Cu²⁺ based on the naphthalimide structure. Chinese Journal of Inorganic Chemistry, 2025, 41(1): 183-192. doi: 10.11862/CJIC.20240232
7. [7]
  Shengfei Dong , Ziyu Liu , Xiaoyi Yang . Hydrothermal liquefaction of biomass for jet fuel precursors: A review. Chinese Chemical Letters, 2024, 35(8): 109142-. doi: 10.1016/j.cclet.2023.109142
8. [8]
  Xiping Dong , Xuan Wang , Zhixiu Lu , Qinhao Shi , Zhengyi Yang , Xuan Yu , Wuliang Feng , Xingli Zou , Yang Liu , Yufeng Zhao . Construction of Cu-Zn Co-doped layered materials for sodium-ion batteries with high cycle stability. Chinese Chemical Letters, 2024, 35(5): 108605-. doi: 10.1016/j.cclet.2023.108605
9. [9]
  Zizhuo Liang , Fuming Du , Ning Zhao , Xiangxin Guo . Revealing the reason for the unsuccessful fabrication of Li3Zr2Si2PO12 by solid state reaction. Chinese Journal of Structural Chemistry, 2023, 42(11): 100108-100108. doi: 10.1016/j.cjsc.2023.100108
10. [10]
  Jing JIN , Zhuming GUO , Zhiyin XIAO , Xiujuan JIANG , Yi HE , Xiaoming LIU . Tuning the stability and cytotoxicity of fac-[Fe(CO)₃I₃]^- anion by its counter ions: From aminiums to inorganic cations. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 991-1004. doi: 10.11862/CJIC.20230458
11. [11]
  Shuangxi Li , Huijun Yu , Tianwei Lan , Liyi Shi , Danhong Cheng , Lupeng Han , Dengsong Zhang . NO_x reduction against alkali poisoning over Ce(SO₄)₂-V₂O₅/TiO₂ catalysts by constructing the Ce⁴⁺–SO₄²⁻ pair sites. Chinese Chemical Letters, 2024, 35(5): 108240-. doi: 10.1016/j.cclet.2023.108240
12. [12]
  Qingyan JIANG , Yanyong SHA , Chen CHEN , Xiaojuan CHEN , Wenlong LIU , Hao HUANG , Hongjiang LIU , Qi LIU . Constructing a one-dimensional Cu-coordination polymer-based cathode material for Li-ion batteries. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 657-668. doi: 10.11862/CJIC.20240004
13. [13]
  Wenhao Chen , Muxuan Wu , Han Chen , Lue Mo , Yirong Zhu . Cu₂Se@C thin film with three-dimensional braided structure as a cathode material for enhanced Cu²⁺ storage. Chinese Chemical Letters, 2024, 35(5): 108698-. doi: 10.1016/j.cclet.2023.108698
14. [14]
  Cuiwu MO , Gangmin ZHANG , Chao WU , Zhipeng HUANG , Chi ZHANG . A(NH₂SO₃) (A=Li, Na): Two ultraviolet transparent sulfamates exhibiting second harmonic generation response. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1387-1396. doi: 10.11862/CJIC.20240045
15. [15]
  Kaimin WANG , Xiong GU , Na DENG , Hongmei YU , Yanqin YE , Yulu MA . Synthesis, structure, fluorescence properties, and Hirshfeld surface analysis of three Zn(Ⅱ)/Cu(Ⅱ) complexes based on 5-(dimethylamino) isophthalic acid. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1397-1408. doi: 10.11862/CJIC.20240009
16. [16]
  Changyuan Bao , Yunpeng Jiang , Haoyin Zhong , Huaizheng Ren , Junhui Wang , Binbin Liu , Qi Zhao , Fan Jin , Yan Meng Chong , Jianguo Sun , Fei Wang , Bo Wang , Ximeng Liu , Dianlong Wang , John Wang . Synergizing 3D-printed structure and sodiophilic interface enables highly efficient sodium metal anodes. Chinese Chemical Letters, 2024, 35(11): 109353-. doi: 10.1016/j.cclet.2023.109353
17. [17]
  Liang Ma , Zhou Li , Zhiqiang Jiang , Xiaofeng Wu , Shixin Chang , Sónia A. C. Carabineiro , Kangle Lv . Effect of precursors on the structure and photocatalytic performance of g-C3N4 for NO oxidation and CO2 reduction. Chinese Journal of Structural Chemistry, 2024, 43(11): 100416-100416. doi: 10.1016/j.cjsc.2024.100416
18. [18]
  Xinzhi Ding , Chong Liu , Jing Niu , Nan Chen , Shutao Xu , Yingxu Wei , Zhongmin Liu . Solid-state NMR study of the stability of MOR framework aluminum. Chinese Journal of Structural Chemistry, 2024, 43(4): 100247-100247. doi: 10.1016/j.cjsc.2024.100247
19. [19]
  Jingyuan Yang , Xinyu Tian , Liuzhong Yuan , Yu Liu , Yue Wang , Chuandong Dou . Enhancing stability of diradical polycyclic hydrocarbons via P=O-attaching. Chinese Chemical Letters, 2024, 35(8): 109745-. doi: 10.1016/j.cclet.2024.109745
20. [20]
  Ting Wang , Xin Yu , Yaqiang Xie . Unlocking stability: Preserving activity of biomimetic catalysts with covalent organic framework cladding. Chinese Chemical Letters, 2024, 35(6): 109320-. doi: 10.1016/j.cclet.2023.109320

Get Citation

PDF

XML

Metrics

PDF Downloads(3)
Abstract views(1114)
HTML views(55)

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

The role of Si coordination structures in the catalytic properties and durability of Cu-SAPO-34 as NH3-SCR catalyst for NOx reduction

Metrics

通讯作者: 陈斌, bchen63@163.com

The role of Si coordination structures in the catalytic properties and durability of Cu-SAPO-34 as NH₃-SCR catalyst for NO_x reduction