Citation: XIE Xing-Xing, FEI Zhao-Yang, ZOU Chong, LI Zheng-Zhou, CHEN Xian, TANG Ji-Hai, CUI Mi-Fen, QIAO Xu. Effects of Rare-Earth Additives on Structures and Performances of CuO-CeO₂-SiO₂ Catalysts for Recycling Cl₂ from HCl Oxidation[J]. Acta Physico-Chimica Sinica, ;2015, 31(6): 1153-1161. doi: 10.3866/PKU.WHXB201504145 shu

Effects of Rare-Earth Additives on Structures and Performances of CuO-CeO₂-SiO₂ Catalysts for Recycling Cl₂ from HCl Oxidation

XIE Xing-Xing ^1,2 ,
FEI Zhao-Yang ^1,2, ,
ZOU Chong ^1,2 ,
LI Zheng-Zhou ^1,2 ,
CHEN Xian ² ,
TANG Ji-Hai ² ,
CUI Mi-Fen ² ,
QIAO Xu ^1,2,

1.
1 State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, P. R. China;
2 College of Chemistry and Chemical Engineering, Nanjing Tech University, Nanjing 210009, P. R. China

Received Date: 23 December 2014
Available Online: 14 April 2015
Fund Project: 国家科技支撑计划(2011BAE18B01) (2011BAE18B01) 江苏省科技支撑计划(BE2011830) (BE2011830) 江苏省高校自然科学基金面上项目(13KJB530006) (13KJB530006) 国家自然科学基金(21306089) (21306089)中国博士后基金(2013M531340)资助 (2013M531340)

CuO-CeO₂-SiO₂ and rare-earth-doped CuO-Ce_0.9M_0.1O₂-SiO₂ (M=La, Pr, Nd) catalysts for recycling Cl₂ from HCl oxidation were prepared by a template method, using activated carbon as a hard template. The catalyst structures were determined using X-ray diffraction (XRD), N₂ adsorption-desorption, transmission electron microscopy (TEM), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and H₂ temperatureprogrammed reduction (H₂-TPR). The catalytic performances were also investigated. The results showed that La, Pr, and Nd cations were incorporated into the CeO₂ lattice and formed nanosized solid solutions; this greatly reduced the catalyst grain sizes, leading to higher surface areas. In addition, the oxygen vacancy concentrations were significantly improved. The changes in the structures and surface properties of the solid solutions significantly affected the HCl catalytic oxidation performances. The order of the activities of various catalysts was CuO-Ce_0.9La_0.1O₂-SiO₂>CuO-Ce_0.9Nd_0.1O₂-SiO₂>CuO-Ce_0.9Pr_0.1O₂-SiO₂>CuO-CeO₂-SiO₂. The oxygen vacancy concentrations of the solid solutions were strongly related to their catalytic activities. However, the structures and performances of the Ce_0.9M_0.1O₂-SiO₂ catalysts showed that an increase in the number of oxygen vacancies resulted in decreased catalytic activities of the solid solutions. Kinetic studies showed that oxygen adsorption could be the rate-determining step for rare-earth-doped catalysts; a higher oxygen vacancy concentration in the solid solution led to a slower reaction rate when the volumetric flow ratio of O₂ to HCl was 1. For the CuOCe_0.9M_0.1O₂-SiO₂ catalysts, spillover of oxygen species in the solid solution into the highly dispersed CuO interfaces was enhanced, which increased the overall reaction rate and gave high activity.
- Rare earth,
- CuO-CeO₂,
- HCl,
- Catalytic oxidation,
- Chlorine,
- Oxygen vacancy
1. [1]
  
  (1) Pérez-Ramírez, J.; Mondelli, C.; Schmidt, T.; Schlüter, O. F. K.; Wolf, A.; Mleczko, L.; Dreier, T. Energy Environ. Sci. 2011, 4, 4786. doi: 10.1039/c1ee02190g
2. [2]
  (2) Deacon, H. Manufacture of Chlorine. U. S. Pat. 85370A, 1868.
3. [3]
  (3) Crihan, D.; Knapp, M.; Zweidinger, S.; Lundgren, E.; Weststrate, C. J.; Andersen, J. N.; Seitsonen A. P.; Over, H. Angew. Chem. Int. Edit. 2008, 47, 2131.
4. [4]
  (4) Tang, J. H.; Chen, X.; Fei, Z. Y.; Zhao, J. H.; Cui, M. F.; Qiao, X. Ind. Eng. Chem. Res. 2013, 52, 11897. doi: 10.1021/ie400200g
5. [5]
  (5) Seki, K. Catal. Surv. Asia 2010, 14, 168. doi: 10.1007/s10563-010-9091-7
6. [6]
  (6) Mondelli, C.; Amrute, A. P.; Krumeich, F.; Schmidit, T.; Pérez- Ramírez, J. ChemCatChem 2011, 3, 657. doi: 10.1002/cctc.201000424
7. [7]
  (7) Mondelli, C.; Amrute, A. P.; Schmidt, T.; Pérez-Ramírez, J. Chem. Commun. 2011, 47, 7173.
8. [8]
  (8) Hernandez, W. Y.; Laguna, O. H.; Centeno, M. A.; Odriozola, J. A. J. Solid State Chem. 2011, 184, 3014. doi: 10.1016/j.jssc.2011.09.018
9. [9]
  (9) Cao, H. Y.; Wang, J. L.; Yan, S. H.; Liu, Z. M.; ng, M. C.; Chen, Y. Q. Acta. Phys. -Chim. Sin. 2012, 28 (8), 1936. [曹红岩, 王健礼, 闫生辉, 刘志敏, 龚茂初, 陈耀强. 物理化学学报, 2012, 28 (8), 1936.] doi: 10.3866/PKU.WHXB201205173
10. [10]
  (10) Wang, S. Y.; Li, N.; Luo, L. F.; Huang, W. X.; Pu, Z. Y.; Wang, J.W.; Hu, G. S.; Luo, M. F.; Lu, J. Q. Appl. Catal. B: Environ. 2014, 144, 325.
11. [11]
  (11) Amrute, A. P.; Mondelli, C.; Moser, M.; Novell-Leruth, G.; López, N.; Rosenthal, D.; Farra, R.; Schüster, M. E.; Teschner, D.; Schmidt, T.; Pérez-Ramírez, J. J. Catal. 2012, 286, 287. doi: 10.1016/j.jcat.2011.11.016
12. [12]
  (12) Moser, M.; Mondelli, C.; Schmidt, T.; Girgsdies, F.; Schüster, M. E.; Farra, R.; Szentmiklósi, L.; Teschner, D.; P rez-Ramírez, J. Appl. Catal. B: Environ. 2013, 132-133, 123.
13. [13]
  (13) Amrute, A. P.; Larrazábal, G. O.; Mondelli, C.; Pérez Ramírez, J. Angew. Chem. Int. Edit. 2013, 52, 9772. doi: 10.1002/ange.201304254
14. [14]
  (14) Chen, X.; Lü, G. M.; Tang, J. H.; Cui, M. F.; Zhou, Z.; Cao, R.; Qiao, X. J. Chem. Eng. Chin. Univ. 2011, 25, 109. [陈献, 吕高明, 汤吉海, 崔咪芬, 周哲, 曹锐, 乔旭. 高校化学工程学报, 2011, 25, 109.]
15. [15]
  (15) Fei, Z. Y.; Liu, H. Y.; Dai, Y.; Ji, W. J.; Chen, X.; Tang, J. H.; Cui, M. F.; Qiao, X. Chem. Eng. J. 2014, 257, 273. doi: 10.1016/j.cej.2014.07.033
16. [16]
  (16) Jampaiah, D.; Tur, K. M.; Ippolito, S. J.; Sabri, Y. M.; Tardio, J.; Bhargava, S. K.; Reddy, B. M. RSC. Adv. 2013, 3, 12963. doi:10.1039/c3ra41441h
17. [17]
  (17) Farra, R.; García-Melchor, M.; Eichelbaum, M.; Hashagen, M.; Frandsen, W.; Allan, J.; Girgsdies, F.; Szentmiklósi, L.; López, N.; Teschner, D. ACS Catal. 2013, 3, 2256. doi: 10.1021/cs4005002
18. [18]
  (18) Jiang, J. T.; Wei, X. J.; Xu, C. Y.; Zhou, Z. X.; Zhen, L. J. Magn. Magn. Mater. 2013, 334, 111. doi: 10.1016/j.jmmm.2012.12.036
19. [19]
  (19) Hernandez, W. Y.; Laguna, O. H.; Centeno, M. A.; Odriozola, J. A. J. Solid State Chem. 2011, 184, 3014. doi: 10.1016/j.jssc.2011.09.018
20. [20]
  (20) Si, R.; Zhang, Y.W.; Li, S. J.; Lin, B. X.; Yan, C. H. J. Phys. Chem. B 2004, 33, 12481.
21. [21]
  (21) Meng, Z. H.; Yang, P.; Zhou, R. X. Acta Phys. -Chim. Sin. 2013, 29 (2), 391. [孟中华, 杨鹏, 周仁贤. 物理化学学报, 2013, 29 (2), 391.] doi: 10.3866/PKU.WHXB201212072
22. [22]
  (22) Yang, D.; Wang, L.; Sun, Y. Z.; Zhou, K. J. Phys. Chem. C 2010, 114, 8926. doi: 10.1021/jp912227p
23. [23]
  (23) Liu, L.; Yao, Z.; Deng, Y.; Gao, F.; Liu, B.; Dong, L. ChemCatChem 2011, 3, 978. doi: 10.1002/cctc.v3.6
24. [24]
  (24) Reddy, B. M.; Saikia, P.; Bharali, P.; Park, S. E.; Muhler, M.; Grüunert, W. J. Phys. Chem. C 2009, 113, 2452. doi: 10.1021/jp809837g
25. [25]
  (25) Katta, L.; Sudarsanam, P.; Thrimurthulu, G.; Reddy, B. M. Appl. Catal. B: Environ. 2010, 101, 101. doi: 10.1016/j.apcatb.2010.09.012
26. [26]
  (26) Gao, X.; Du, X. S.; Cui, L.W.; Fu, Y. C.; Luo, Z. Y.; Cen, K. F. Catal. Commun. 2010, 12, 255.
27. [27]
  (27) Menon, U.; Poelman, H.; Bliznuk, V.; Galvita, V. V.; Poelman, D.; Marin, G. B. J. Catal. 2012, 295, 91. doi: 10.1016/j.jcat.2012.07.026
28. [28]
  (28) Amrute, A. P.; Mondelli, C.; Miguel, A. G.; Hevia, P. J. J. Phys. Chem. C 2011, 115, 1056.
29. [29]
  (29) Farra, R.; Wrabetz, S.; Schuster, E. S.; Stotz, E.; Hamilton, N. G.; Amrute, A. P.; Pérez-Ramírez, J.; López, N.; Teschner, D. Phys. Chem. Chem. Phys. 2013, 15, 3454. doi: 10.1039/c2cp42767b
1. [1]
  Yongmei Liu , Lisen Sun , Zhen Huang , Tao Tu . Curriculum-Based Ideological and Political Design for the Experiment of Methanol Oxidation to Formaldehyde Catalyzed by Electrolytic Silver. University Chemistry, 2024, 39(2): 67-71. doi: 10.3866/PKU.DXHX202308020
2. [2]
  Chunchun Wang , Changjun You , Ke Rong , Chuqi Shen , Fang Yang , Shijie Li . An S-Scheme MIL-101(Fe)-on-BiOCl Heterostructure with Oxygen Vacancies for Boosting Photocatalytic Removal of Cr(Ⅵ). Acta Physico-Chimica Sinica, 2024, 40(7): 2307045-0. doi: 10.3866/PKU.WHXB202307045
3. [3]
  Weicheng Feng , Jingcheng Yu , Yilan Yang , Yige Guo , Geng Zou , Xiaoju Liu , Zhou Chen , Kun Dong , Yuefeng Song , Guoxiong Wang , Xinhe Bao . Regulating the High Entropy Component of Double Perovskite for High-Temperature Oxygen Evolution Reaction. Acta Physico-Chimica Sinica, 2024, 40(6): 2306013-0. doi: 10.3866/PKU.WHXB202306013
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): 2407005-0. doi: 10.3866/PKU.WHXB202407005
5. [5]
  Wenlong LI , Xinyu JIA , Jie LING , Mengdan MA , Anning ZHOU . Photothermal catalytic CO₂ hydrogenation over a Mg-doped In₂O_3-x catalyst. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 919-929. doi: 10.11862/CJIC.20230421
6. [6]
  Huafeng SHI . Construction of MnCoNi layered double hydroxide@Co-Ni-S amorphous hollow polyhedron composite with excellent electrocatalytic oxygen evolution performance. Chinese Journal of Inorganic Chemistry, 2025, 41(7): 1380-1386. doi: 10.11862/CJIC.20240378
7. [7]
  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
8. [8]
  Wang Wang , Yucheng Liu , Shengli Chen . Use of NiFe Layered Double Hydroxide as Electrocatalyst in Oxygen Evolution Reaction: Catalytic Mechanisms, Electrode Design, and Durability. Acta Physico-Chimica Sinica, 2024, 40(2): 2303059-0. doi: 10.3866/PKU.WHXB202303059
9. [9]
  Liu Lin , Zemin Sun , Huatian Chen , Lian Zhao , Mingyue Sun , Yitao Yang , Zhensheng Liao , Xinyu Wu , Xinxin Li , Cheng Tang . Recent Advances in Electrocatalytic Two-Electron Water Oxidation for Green H₂O₂ Production. Acta Physico-Chimica Sinica, 2024, 40(4): 2305019-0. doi: 10.3866/PKU.WHXB202305019
10. [10]
  Chuanming GUO , Kaiyang ZHANG , Yun WU , Rui YAO , Qiang ZHAO , Jinping LI , Guang LIU . Performance of MnO₂-0.39IrO_x composite oxides for water oxidation reaction in acidic media. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1135-1142. doi: 10.11862/CJIC.20230459
11. [11]
  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
12. [12]
  Ke Li , Chuang Liu , Jingping Li , Guohong Wang , Kai Wang . Architecting Inorganic/Organic S-Scheme Heterojunction of Bi₄Ti₃O₁₂ Coupling with g-C₃N₄ for Photocatalytic H₂O₂ Production from Pure Water. Acta Physico-Chimica Sinica, 2024, 40(11): 2403009-0. doi: 10.3866/PKU.WHXB202403009
13. [13]
  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
14. [14]
  Endong YANG , Haoze TIAN , Ke ZHANG , Yongbing LOU . Efficient oxygen evolution reaction of CuCo₂O₄/NiFe-layered bimetallic hydroxide core-shell nanoflower sphere arrays. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 930-940. doi: 10.11862/CJIC.20230369
15. [15]
  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
16. [16]
  Yinjie Xu , Suiqin Li , Lihao Liu , Jiahui He , Kai Li , Mengxin Wang , Shuying Zhao , Chun Li , Zhengbin Zhang , Xing Zhong , Jianguo Wang . Enhanced Electrocatalytic Oxidation of Sterols using the Synergistic Effect of NiFe-MOF and Aminoxyl Radicals. Acta Physico-Chimica Sinica, 2024, 40(3): 2305012-0. doi: 10.3866/PKU.WHXB202305012
17. [17]
  Hailang JIA , Pengcheng JI , Hongcheng LI . Preparation and performance of nickel doped ruthenium dioxide electrocatalyst for oxygen evolution. Chinese Journal of Inorganic Chemistry, 2025, 41(8): 1632-1640. doi: 10.11862/CJIC.20240398
18. [18]
  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
19. [19]
  Yu Dai , Xueting Sun , Haoyu Wu , Naizhu Li , Guoe Cheng , Xiaojin Zhang , Fan Xia . Determination of the Michaelis Constant for Gold Nanozyme-Catalyzed Decomposition of Hydrogen Peroxide. University Chemistry, 2025, 40(5): 351-356. doi: 10.12461/PKU.DXHX202407052
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(317)
Abstract views(882)
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

Effects of Rare-Earth Additives on Structures and Performances of CuO-CeO2-SiO2 Catalysts for Recycling Cl2 from HCl Oxidation

Metrics

通讯作者: 陈斌, bchen63@163.com

Effects of Rare-Earth Additives on Structures and Performances of CuO-CeO₂-SiO₂ Catalysts for Recycling Cl₂ from HCl Oxidation