Citation: FAN Feng-Qi, MENG Ming, TIAN Ye, ZHENG Li-Rong, ZHANG Jing, HU Tian-Dou. Effect of Cu Loading on the Structure and Catalytic Performance of the LNT Catalyst CuO-K₂CO₃/TiO₂[J]. Acta Physico-Chimica Sinica, ;2015, 31(9): 1761-1770. doi: 10.3866/PKU.WHXB201507291 shu

Effect of Cu Loading on the Structure and Catalytic Performance of the LNT Catalyst CuO-K₂CO₃/TiO₂

1.
1 Collaborative Innovation Center of Chemical Science and Engineering Tianjin, Tianjin Key Laboratory of Applied Catalysis Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, P. R. China;
2 Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, P. R. China

Received Date: 17 April 2015
Available Online: 29 July 2015
Fund Project: 国家自然科学基金(21276184, U1332102, 21476160) (21276184, U1332102, 21476160) 高等学校博士学科点专项科研基金(20120032110014) (20120032110014) 天津市自然科学基金(12JCYBJC14000, 15JCZDJC37400) (12JCYBJC14000, 15JCZDJC37400)中国大学学科人才引进计划(B06006)资助 (B06006)

A series of non-platinic lean NO_x trap (LNT) CuO-K₂CO₃/TiO₂ catalysts with different Cu loadings were prepared by sequential impregnation, and they showed relatively od performance for lean NO_x storage and reduction. The catalyst containing 8% (w) CuO showed not only the largest NO_x storage capacity of 1.559 mmol·g^-1 under lean conditions, but also the highest NO_x reduction percentage of 99% in cyclic lean/rich atmospheres. Additionally, zero selectivity of NO_x to N₂O was achieved over this catalyst during NO_x reduction. Multiple techniques, including X-ray diffraction (XRD), high-resolution transmission electron microscopy (HR-TEM), temperature-programmed desorption of CO₂ (CO₂-TPD), extended X-ray absorption fine structure (EXAFS), temperature-programmed reduction of H₂ (H₂-TPR), and in-situ diffuse reflectance Fourier-transform infrared spectroscopy (DRIFTS), were used for catalyst characterization. The results indicate that highly dispersed CuO is the main active phase for oxidation of NO to NO₂ and reduction of NO_x to N₂. The strong interaction between K₂CO₃ and CuO was clearly revealed, which favors NO_x adsorption and storage. The appearance of negative bands at around 1436 and 1563 cm^-1, corresponding to CO₂ asymmetric stretching in bicarbonates and -C=O stretching in bidentate carbonates, showed the involvement of carbonates in NO_x storage. After using the catalysts for 15 cycles of NO_x storage and reduction in alternative lean/rich atmospheres, the CuO species in the catalysts showed little change, indicating high catalytic stability. Based on the results of in-situ DRIFTS and the other characterizations, a model describing the NO_x storage processes and the distribution of CuO and K₂CO₃ species is proposed.
- NO_x,
- Storage,
- Reduction,
- Copper oxide,
- Potassium carbonate
1. [1]
  
  (1) Roy, S.; Baiker, A. Chem. Rev. 2009, 109, 4054. doi: 10.1021/cr800496f
2. [2]
  (2) Klingstedt, F.; Arve, K.; Eränen, K.; Murzin, D. Y. Accounts Chem. Res. 2006, 39, 273. doi: 10.1021/ar050185k
3. [3]
  (3) Takahashi, N.; Shinjoh, H.; Iijima, T.; Suzuki, T.; Yamazaki, K.; Yokota, K.; Suzuki, H.; Miyoshi, N.; Matsumoto, S.; Tanizawa, T.; Tanaka, T.; Tateishi, S.; Kasahara, K. Catal. Today 1996, 27, 63.
4. [4]
  (4) Xian, H.; Ma, A. J.; Meng, M.; Li, X. G. Acta Phys. -Chim. Sin. 2013, 29, 2437. [贤晖, 马爱静, 孟明, 李新刚. 物理化学学报, 2013, 29, 2437.] doi: 10.3866/PKU.WHXB201309052
5. [5]
  (5) Hadjiivanov, K.; Klissurski, D.; Ramis, G.; Busca, G. Appl. Catal. B 1996, 7, 251. doi: 10.1016/0926-3373(95)00034-8
6. [6]
  (6) Sultana, A.; Haneda, M.; Hamada, H. Appl. Catal. B 2009, 88, 180. doi: 10.1016/j.apcatb.2008.08.028
7. [7]
  (7) Zhang, W. X.; Yahiro, H.; Mizuno, N.; Izumi, J.; Iwamoto, M. Langmuir 1993, 9, 2337. doi: 10.1021/la00033a015
8. [8]
  (8) Liu, J.; Li, X. Y.; Zhao, Q. D.; Zhang, D. K.; Ndokoye, P. J. Mol. Catal. A 2013, 378, 115.
9. [9]
  (9) Guerrero, S.; Guzmán, I.; Aguila, G.; Chornik, B.; Araya, P. Appl. Catal. B 2012, 123-124, 282.
10. [10]
  (10) Glisenti, A.; Natile, M. M.; Carlotto, S.; Vittadini, A. Catal. Lett. 2014, 144, 1466.
11. [11]
  (11) Matsumoto, S. I.; Ikeda, Y.; Suzuki, H.; Ogai, M.; Miyoshi, N. Appl. Catal. B 2000, 25, 115. doi: 10.1016/S0926-3373(99) 00124-1
12. [12]
  (12) Frola, F.; Manzoli, M.; Prinetto, F.; Ghiotti, G.; Castoldi, L.; Lietti, L. J. Phys. Chem. C 2008, 112, 12869. doi: 10.1021/jp801480t
13. [13]
  (13) Lietti, L.; Forzatti, P.; Nova, I.; Tronconi, E. J. Catal. 2001, 204, 175. doi: 10.1006/jcat.2001.3370
14. [14]
  (14) Nova, I.; Castoldi, L.; Lietti, L.; Tronconi, E.; Forzatti, P.; Prinetto, F.; Ghiotti, G. J. Catal. 2004, 222, 377. doi: 10.1016/j.jcat.2003.11.013
15. [15]
  (15) Delucasconsuegra, A.; Caravaca, A.; Sanchez, P.; Dorado, F.; Valverde, J. J. Catal. 2008, 259, 54.
16. [16]
  (16) Shen, W. H.; Nitta, A.; Chen, Z.; Eda, T.; Yoshida, A.; Naito, S. C. J. Catal. 2011, 280, 161. doi: 10.1016/j.jcat.2011.03.014
17. [17]
  (17) Castoldi, L.; Lietti, L.; Forzatti, P.; Morandi, S.; Ghiotti, G.; Vindigni, F. J. Catal. 2010, 276, 335. doi: 10.1016/j.jcat. 2010.09.026
18. [18]
  (18) Liu, Y.; Meng, M.; Li, X. G.; Guo, L. H.; Zha, Y. Q. Chem. Eng. Res. Des. 2008, 86, 932. doi: 10.1016/j.cherd.2008.02.010
19. [19]
  (19) Hou, N. N.; Zhang, Y. X.; Meng, M. J. Phys. Chem. C 2013, 117, 4089.
20. [20]
  (20) Li, W. B.; Yang, R. T.; Krist, K.; Regalbuto, J. R. Energ. Fuel 1997, 11, 428. doi: 10.1021/ef960128v
21. [21]
  (21) Huang, J.; Wang, S. R.; Zhao, Y. Q.; Wang, X. Y.; Wang, S. P.; Wu, S. H.; Zhang, S. M.; Huang, W. P. Catal. Commun. 2006, 7, 1029. doi: 10.1016/j.catcom.2006.05.001
22. [22]
  (22) Chen, C. S.; Chen, T. C.; Chen, C. C.; Lai, Y. T.; You, J. H.; Chou, T. M.; Chen, C. H.; Lee, J. F. Langmuir 2012, 28, 9996.
23. [23]
  (23) You, R.; Zhang, Y. X; Liu, D. S.; Meng, M.; Zheng, L. R.; Zhang, J.; Hu, T. D. J. Phys. Chem. C 2014, 118, 25403. doi: 10.1021/jp505601x
24. [24]
  (24) Wang, Q.; Sohn, J. H.; Chung, J. S. Appl. Catal. B 2009, 89, 97. doi: 10.1016/j.apcatb.2008.12.007
25. [25]
  (25) Li, Z. B.; Meng, M.; You, R.; Ding, T.; Li, Z. J. Catal. Lett. 2012, 142, 1067. doi: 10.1007/s10562-012-0864-7
26. [26]
  (26) Zhang, L. J.; Cui, S. P.; Guo, H. X.; Ma, X. Y.; Luo, X. G. J. Mol. Catal. A 2014, 390, 14. doi: 10.1016/j.molcata.2014.02.021
27. [27]
  (27) Zhang, Y. X.; Meng, M.; Dai, F. F.; Ding, T.; You, R. J. Phys. Chem. C 2013, 117, 23691. doi: 10.1021/jp406950u
28. [28]
  (28) Friedman, R. M.; Freeman, J. J.; Lytle, F. W. J. Catal. 1978, 55, 10. doi: 10.1016/0021-9517(78)90181-1
29. [29]
  (29) Liu, W.; Flytzani-Stephanopoulos, M. Chem. Eng. J. 1996, 64, 283.
30. [30]
  (30) Bhuiyan, M. M. R.; Lin, S. D.; Hsiao, T. C. Catal. Today 2014, 226, 150. doi: 10.1016/j.cattod.2013.10.053
31. [31]
  (31) Fox, E. B.; Velu, S.; Engelhard, M. H.; Chin, Y. H.; Miller, J. T.; Kropf, J.; Song, C. J. Catal. 2008, 260, 358. doi: 10.1016/j.jcat. 2008.08.018
32. [32]
  (32) Zhang, Y. X.; Liu, D. S.; Meng, M.; Jiang, Z.; Zhang, S. Ind. Eng. Chem. Res. 2014, 53, 8416. doi: 10.1021/ie501034u
33. [33]
  (33) Chen, L. F.; Guo, P. J.; Qiao, M. H.; Yan, S. R.; Li, H. X.; Shen, W.; Xu, H. L.; Fan, K. N. J. Catal. 2008, 257, 172. doi: 10.1016/j.jcat.2008.04.021
34. [34]
  (34) Prinetto, F.; Manzoli, M.; Morandi, S.; Frola, F.; Ghiotti, G.; Castoldi, L.; Lietti, L.; Forzatti, P. J. Phys. Chem. C 2009, 114, 1127.
35. [35]
  (35) Toops, T. J.; Smith, D. B.; Partridge, W. P. Appl. Catal. B 2005, 58, 245. doi: 10.1016/j.apcatb.2004.10.021
36. [36]
  (36) Prinetto, F.; Ghiotti, G.; Nova, I.; Lietti, L.; Tronconi, E.; Forzatti, P. J. Phys. Chem. B 2001, 105, 12732. doi: 10.1021/jp012702w
37. [37]
  (37) Montanari, T.; Castoldi, L.; Lietti, L.; Busca, G. Appl. Catal. A 2011, 400, 61. doi: 10.1016/j.apcata.2011.04.016
38. [38]
  (38) Fanson, P. T.; Horton, M. R.; Delgass, W. N.; Lauterbach, J. Appl. Catal. B 2003, 46, 393. doi: 10.1016/S0926-3373(03) 00275-3
39. [39]
  (39) Qi, G. S.; Li, W. Catal. Lett. 2013, 144, 639.
1. [1]
  Shanyuan Bi , Jin Zhang , Dengchao Peng , Danhong Cheng , Jianping Zhang , Lupeng Han , Dengsong Zhang . Improved N₂ selectivity for low-temperature NO_x reduction over etched ZSM-5 supported MnCe oxide catalysts. Chinese Chemical Letters, 2025, 36(5): 110295-. doi: 10.1016/j.cclet.2024.110295
2. [2]
  Jianning Zhang , Yihuai Zhang , Guoxin Ma , Jingchen Zhao , Tao Zhang , Jian Liu . Enhancing hydrothermal stability in Cu/SSZ-13 catalyst for diesel SCR applications through a novel core-shell structure. Chinese Chemical Letters, 2025, 36(7): 110516-. doi: 10.1016/j.cclet.2024.110516
3. [3]
  Zhuoya WANG , Le HE , Zhiquan LIN , Yingxi WANG , Ling LI . Multifunctional nanozyme Prussian blue modified copper peroxide: Synthesis and photothermal enhanced catalytic therapy of self-provided hydrogen peroxide. Chinese Journal of Inorganic Chemistry, 2024, 40(12): 2445-2454. doi: 10.11862/CJIC.20240194
4. [4]
  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
5. [5]
  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
6. [6]
  Hui Shi , Shuangyan Huan , Yuzhi Wang . Ideological and Political Design of Potassium Permanganate Oxidation-Reduction Titration Experiment. University Chemistry, 2024, 39(2): 175-180. doi: 10.3866/PKU.DXHX202308042
7. [7]
  Tong Zhou , Jun Li , Zitian Wen , Yitian Chen , Hailing Li , Zhonghong Gao , Wenyun Wang , Fang Liu , Qing Feng , Zhen Li , Jinyi Yang , Min Liu , Wei Qi . Experiment Improvement of “Redox Reaction and Electrode Potential” Based on the New Medical Concept. University Chemistry, 2024, 39(8): 276-281. doi: 10.3866/PKU.DXHX202401005
8. [8]
  Ji-Quan Liu , Huilin Guo , Ying Yang , Xiaohui Guo . Calculation and Discussion of Electrode Potentials in Redox Reactions of Water. University Chemistry, 2024, 39(8): 351-358. doi: 10.3866/PKU.DXHX202401031
9. [9]
  Zhihuan XU , Qing KANG , Yuzhen LONG , Qian YUAN , Cidong LIU , Xin LI , Genghuai TANG , Yuqing LIAO . Effect of graphene oxide concentration on the electrochemical properties of reduced graphene oxide/ZnS. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1329-1336. doi: 10.11862/CJIC.20230447
10. [10]
  Zhuo Wang , Xue Bai , Kexin Zhang , Hongzhi Wang , Jiabao Dong , Yuan Gao , Bin Zhao . MOF-Templated Synthesis of Nitrogen-Doped Carbon for Enhanced Electrochemical Sodium Ion Storage and Removal. Acta Physico-Chimica Sinica, 2025, 41(3): 2405002-0. doi: 10.3866/PKU.WHXB202405002
11. [11]
  Qiang Zhang , Yuanbiao Huang , Rong Cao . Imidazolium-Based Materials for CO₂ Electroreduction. Acta Physico-Chimica Sinica, 2024, 40(4): 2306040-0. doi: 10.3866/PKU.WHXB202306040
12. [12]
  Zilin Hu , Yaoshen Niu , Xiaohui Rong , Yongsheng Hu . Suppression of Voltage Decay through Ni³⁺ Barrier in Anionic-Redox Active Cathode for Na-Ion Batteries. Acta Physico-Chimica Sinica, 2024, 40(6): 2306005-0. doi: 10.3866/PKU.WHXB202306005
13. [13]
  Zhaoyu Wen , Na Han , Yanguang Li . Recent Progress towards the Production of H₂O₂ by Electrochemical Two-Electron Oxygen Reduction Reaction. Acta Physico-Chimica Sinica, 2024, 40(2): 2304001-0. doi: 10.3866/PKU.WHXB202304001
14. [14]
  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
15. [15]
  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
16. [16]
  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
17. [17]
  Tingting Jiang , Jing Chang . Application of Ideological and Political Education in Chemical Analysis Experiment under the Background of Emerging Engineering Education: Taking the Redox Titration Experiment as an Example. University Chemistry, 2024, 39(2): 168-174. doi: 10.3866/PKU.DXHX202308007
18. [18]
  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
19. [19]
  Lisha LEI , Wei YONG , Yiting CHENG , Yibo WANG , Wenchao HUANG , Junhuan ZHAO , Zhongjie ZHAI , Yangbin DING . Application of regenerated cellulose and reduced graphene oxide film in synergistic power generation from moisture electricity generation and Mg-air batteries. Chinese Journal of Inorganic Chemistry, 2025, 41(6): 1151-1161. doi: 10.11862/CJIC.20240202
20. [20]
  Jianan Hong , Chenyu Xu , Yan Liu , Changqi Li , Menglin Wang , Yanwei Zhang . Decoding the interfacial competition between hydrogen evolution and CO₂ reduction via edge-active-site modulation in photothermal catalysis. Acta Physico-Chimica Sinica, 2025, 41(9): 100099-0. doi: 10.1016/j.actphy.2025.100099

Get Citation

PDF

XML

Metrics

PDF Downloads(183)
Abstract views(722)
HTML views(39)

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

Effect of Cu Loading on the Structure and Catalytic Performance of the LNT Catalyst CuO-K2CO3/TiO2

Metrics

通讯作者: 陈斌, bchen63@163.com

Effect of Cu Loading on the Structure and Catalytic Performance of the LNT Catalyst CuO-K₂CO₃/TiO₂