Citation: TANG Hao, LU Qiang, YANG Jiang-yi, LI Hui, LI Wen-yan, YANG Yong-ping. Research on recycling and characterization analysis of the waste SCR catalyst[J]. Journal of Fuel Chemistry and Technology, ;2018, 46(2): 233-242. shu

Research on recycling and characterization analysis of the waste SCR catalyst

National Engineering Laboratory for Biomass Power Generation Equipment, North China Electric Power University, Beijing 102206, China

Corresponding author: LU Qiang, qianglu@mail.ustc.edu.cn.
Received Date: 30 August 2017
Revised Date: 16 December 2017

Fund Project: Fundamental Research Funds for the Central Universities 2015ZZD02the Major State Basic Research Development Program of China 2015CB251501the Major State Basic Research Development Program of China 973 projectThe project was supported by the Major State Basic Research Development Program of China (973 project, 2015CB251501), Beijing Nova Program (Z171100001117064) and Fundamental Research Funds for the Central Universities (2016YQ05, 2015ZZD02)Fundamental Research Funds for the Central Universities 2016YQ05Beijing Nova Program Z171100001117064

Figures(10)

In the light of a high SO₂ oxidation ratio of the recycled waste SCR catalyst during conventional recycling denitrification, a novel recycling technique, including acid washing, acid leaching under reduction condition and active components loading, was proposed to control the SO₂ oxidation ratio of the recycled catalyst.The experiments were performed to determine the components, denitrification efficiency and SO₂ oxidation ratio of the catalysts obtained in different recycling runs, and the catalysts used were characterized.The results indicate that the denitrification efficiency and SO₂ oxidation ratio of the fresh catalyst, waste catalyst, conventional recycled catalyst and novel recycled catalyst are 99.0% and 0.43%, 77.0% and 0.46%, 94.2% and 0.80%, 99.3% and 0.48%, respectively.Through novel recycling method, both denitrification efficiency and SO₂ oxidation ratio of the recycled catalyst are well recovered.The characterization results suggest that the highly polymerized vanadium species on the surface of the waste catalyst could not be removed by using conventional recycling method, but the novel recycling method is effective for removing these vanadium species and replacing them with highly dispersed vanadium species, resulting in a reduction of SO₂ oxidation ratio of the recycled catalyst.
- catalyst,
- waste,
- recycling,
- SO₂ oxidation
1. [1]
  HUANG Zeng-bin, LI Cui-qing, WANG Zhen, XU Sheng-mei, FENG Ling-bo, WANG Hong, SONG Yong-ji, ZHANG Wei. Performance of Mn-Ce catalysts supported on different zeolites in the NH₃-SCR of NO_x[J]. J Fuel Chem Technol, 2016,44(11):495-499.
2. [2]
  SHANG Xue-song, CHEN Jin-sheng, ZHAO Jin-ping, ZHANG Fu-wang, XU Ya, XU Qi. Discussion on the deactivation of SCR denitrification catalyst and its reasons[J]. J Fuel Chem Technol, 2011,39(6):465-470.
3. [3]
  HUO Y T, CHANG Z D, LI W J, LIU S X, DONG B. Reuse and valorization of vanadium and tungsten from waste V₂O₅-WO₃/TiO₂ SCR catalyst[J]. Waste Biomass Valor, 2015,6(2):159-165. doi: 10.1007/s12649-014-9335-2
4. [4]
  ZHAO Z P, GUO M, ZHANG M. Extraction of molybdenum and vanadium from the spent diesel exhaust catalyst by ammonia leaching method[J]. J Hazard Mater, 2015,286:402-409. doi: 10.1016/j.jhazmat.2014.12.063
5. [5]
  CHEN Chen, LU Qiang, LIN Zhuo-wei, LI Wen-yan, DONG Chang-qing. Research progress of element recovery of waste De-NO_x SCR catalyst from coal-fired power plants[J]. Chem Ind Eng Prog, 2016,35(10):3306-3312.
6. [6]
  LEE J B, LEE T W, SONG K C, LEE I Y. Method of regenerating honeycomb type SCR catalyst by air lift loop reactor: US, 2006/0094587A1[P]. 2006-05-04.
7. [7]
  SHI Wei-wei. Impregnation regeneration and SO₂ oxidation control of the SCR denitrification catalysts[D]. Guangzhou: South China University of Technology, 2013.
8. [8]
  LIU Jian-hua. Regeneration and SO₂ oxidation control of plate-type SCR denitrification catalysts[D]. Guangzhou: South China University of Technology, 2016.
9. [9]
  MENASHA J, DUNN-RANKIN D, MUZIO L, STALLINGS J. Ammonium bisulfate formation temperature in a bench-scale single-channel air preheater[J]. Fuel, 2011,90(7):2445-2453. doi: 10.1016/j.fuel.2011.03.006
10. [10]
  YAKHNIN V Z, MENZINGER M. Deactivation avalanches through the interaction of locally deactivated catalyst with traveling hot spots[J]. Stud Surf Sci Catal, 1999,126:291-298. doi: 10.1016/S0167-2991(99)80478-9
11. [11]
  DUNN J P, STENGER H G, WACHS I E. Oxidation of SO₂ over supported metal oxide catalysts[J]. J Catal, 1999,181(2):233-243. doi: 10.1006/jcat.1998.2305
12. [12]
  ORSENIGO, LIETTI, TRONCONI, FORZATTI, BREGANI. Dynamic investigation of the role of the surface sulfates in NO_x reduction and SO₂ oxidation over DeNO_x-SCR catalysts[J]. Ind Eng Chem Res, 1998,165(37):2350-2359.
13. [13]
  LIU X S, WU X D, XU T F, WENG D, SI Z C, RAN R. Effects of silica additive on the NH₃-SCR activity and thermal stability of a V₂O₅/WO₃-TiO₂ catalyst[J]. Chin J Catal, 2016,37(8):1340-1346. doi: 10.1016/S1872-2067(15)61109-3
14. [14]
  XU Hao, YAN Wei, YOU Li. Effects of various acids treatment on the properties of titanium substrate[J]. Rare Met Mater Eng, 2011,40(9):1550-1554.
15. [15]
  LIU Jun, WANG Liang-liang, FEI Zhao-yang, CHEN Xian, TANG Ji-hai, CUI Mi-fen, QIAO Xu. Structure and properties of amorphous CeO₂@TiO₂ catalyst and its performance in the selective catalytic reduction of NO with NH₃[J]. J Fuel Chem Technol, 2016,44(8):954-960.
16. [16]
  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. Low-temperature selective catalytic reduction of NO with NH₃ over nanoflaky MnO_x on carbon nanotubes in situ prepared via a chemical bath deposition route[J]. Nanoscale, 2013,05(19):9199-9207. doi: 10.1039/c3nr02631k
17. [17]
  RAMIS G, BUSCA G, LORENZELLL V. Spectroscopic characterization of magnesium vanadate catalysts. Part 2. FTIR study of the surface properties of pure and mixed-phase powders[J]. J Chem Soc Faraday Trans, 1994,90(9):1293-1299. doi: 10.1039/FT9949001293
18. [18]
  LIU X, LI J H, LI X, PENG Y, WANG H, JIANG X M, WANG L W. NH₃ selective catalytic reduction of NO:A large surface TiO₂ support and its promotion of V₂O₅ dispersion on the prepared catalyst[J]. Chin J Catal, 2016,37(6):878-887. doi: 10.1016/S1872-2067(15)61041-5
19. [19]
  PENG Y, LI J H, SI W Z, LUO J M, WANG Y, JIE F, LI X, CRITTENDEN J, HAO J M. Deactivation and regeneration of a commercial SCR catalyst:Comparison with alkali metals and arsenic[J]. Appl Catal B:Environ, 2015,168-169:195-202. doi: 10.1016/j.apcatb.2014.12.005
20. [20]
  LI Q C, CHEN S F, LIU Z Y, LIU Q Y. Combined effect of KCl and SO₂ on the selective catalytic reduction of NO by NH₃ over V₂O₅/TiO₂ catalyst[J]. Appl Catal B:Environ, 2015,164:475-482. doi: 10.1016/j.apcatb.2014.09.036
21. [21]
  DONG G J, ZHANG Y F, ZHAO Y, BAI Y. Effect of the pH value of precursor solution on the catalytic performance of V₂O₅-WO₃/TiO₂ in the low temperature NH₃-SCR of NO_x[J]. J Fuel Chem Technol, 2014,42(12):1455-1463. doi: 10.1016/S1872-5813(15)60003-2
22. [22]
  YANG Jian, LIN Fan, CHEN Kui, KONG Ming, ZHAO Dong, MENG Fei. Activity and SO₂ deactivation mechanism of vanadium series catalyst containing cerium[J]. J Fuel Chem Technol, 2016,44(11):1394-1400. doi: 10.3969/j.issn.0253-2409.2016.11.017
23. [23]
  SHEN Bo-xiong, LU Feng-ju, GAO Lan-jun, YUE Shi-ji. Study on alkali and alkaline earths poisoning characteristics for a commercial SCR catalyst[J]. J Fuel Chem Technol, 2011,44(4):500-506.
24. [24]
  LIU J, LI X Y, ZHAO Q D, KE J, XIAO H N, LV X J, LIU S M, TADÉ M, WANG S B. Mechanistic investigation of the enhanced NH₃-SCR on cobalt-decorated Ce-Ti mixed oxide:In situ, FT-IR analysis for structure-activity correlation[J]. Appl Catal B:Environ, 2017,200:297-308. doi: 10.1016/j.apcatb.2016.07.020
25. [25]
  SHEN Bo-xiong, XIONG Li-xian, LIU Ting, WANG Jing, TIAN Xiao-juan. Alkali deactivation and regeneration of nano V₂O₅-WO₃/TiO₂ catalysts[J]. J Fuel Chem Technol, 2010,38(1):85-90.
26. [26]
  ZHAO H, BENNICI S, SHEN J, AUROUX A. The influence of the preparation method on the structural, acidic and redox properties of V₂O₅-TiO₂/SO₄^2- catalysts[J]. Appl Catal A:Gen, 2009,356(2):121-128. doi: 10.1016/j.apcata.2008.12.037
27. [27]
  EL-MAAZAWI M, FINKEN A N, NAIR A B, GRASSIAN V H. Adsorption and photocatalytic oxidation of acetone on TiO₂:An in situ transmission FT-IR study[J]. J Catal, 2000,191(1):138-146. doi: 10.1006/jcat.1999.2794
28. [28]
  JIANG Ye, GAO Xiang, DU Xue-sen, MAO Jian-hong, LUO Zhong-yang, CEN Ke-fa. The effect of PbO on a V₂O₅/TiO₂ catalyst for selective catalytic reduction on NO with NH₃[J]. J Eng Thermophys, 2009,30(11):1973-1976. doi: 10.3321/j.issn:0253-231X.2009.11.048
29. [29]
  CHEN J P, YANG R T. Selective catalytic reduction of NO with NH₃ on SO₄^2-/TiO₂ superacid catalyst[J]. J Catal, 1993,139(1):277-288. doi: 10.1006/jcat.1993.1023
30. [30]
  SHANG X S, HU G R, HE C, ZHAO J P, ZHANG F W, XU Y, ZHANG Y F, LI J R, CHEN J S. Regeneration of full-scale commercial honeycomb monolith catalyst (V₂O₅-WO₃/TiO₂) used in coal-fired power plant[J]. J Ind and Eng Chem, 2012,18(1):513-519. doi: 10.1016/j.jiec.2011.11.070
31. [31]
  KONG Ming, LIU Qing-cai, ZHAO Dong, REN Shan, MENG Fei. Synergy of NaCl and Hg⁰ on V₂O₅-WO₃/TiO₂ SCR catalysts[J]. J Fuel Chem Technol, 2015,43(12):1504-1509. doi: 10.3969/j.issn.0253-2409.2015.12.015
1. [1]
  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
2. [2]
  Jiayi Yang , Jianxiu Hao , Huacong Zhou , Quansheng Liu . “Gorgeous Transformation” of Carbon Dioxide into Cyclic Carbonates: Catalyst Types and Roles. University Chemistry, 2026, 41(2): 178-189. doi: 10.12461/PKU.DXHX202502105
3. [3]
  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
4. [4]
  Wentao Xu , Xuyan Mo , Yang Zhou , Zuxian Weng , Kunling Mo , Yanhua Wu , Xinlin Jiang , Dan Li , Tangqi Lan , Huan Wen , Fuqin Zheng , Youjun Fan , Wei Chen . Bimetal Leaching Induced Reconstruction of Water Oxidation Electrocatalyst for Enhanced Activity and Stability. Acta Physico-Chimica Sinica, 2024, 40(8): 2308003-0. doi: 10.3866/PKU.WHXB202308003
5. [5]
  Chenyang WANG , Yiyan BAI , Wei ZHANG , Zhaorong LIU , Yuchun WANG . Performance of photo-assisted copper oxide catalyzed hydrolysis of ammonia borane to produce hydrogen. Chinese Journal of Inorganic Chemistry, 2026, 42(1): 97-110. doi: 10.11862/CJIC.20250116
6. [6]
  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
7. [7]
  Mei-Xia Yang , Zhen-Hong He , Long-Rui Wang , You-Xing Yang . Route for Turning Waste CH₄ and CO₂ into Valuable Products: Reforming for Syngas. University Chemistry, 2026, 41(2): 197-207. doi: 10.12461/PKU.DXHX202503012
8. [8]
  Wenruo NI , Hongpeng LI , Yun ZHANG , Yiran TIAN , Jiehui RUI , Yingcheng TONG , Xiaolin PI , Zhenyan TANG . Research progress of ruthenium alloy catalysts in hydrogen evolution reaction. Chinese Journal of Inorganic Chemistry, 2026, 42(1): 23-44. doi: 10.11862/CJIC.20250188
9. [9]
  Shuting KONG , Fengshi ZHANG , Zhiyi LU , Yanling LIU , Minglang YE , Zhengfang HU , Longsheng WANG , Bing HU , Haiying WANG . Research advance of the preparation of tributyl citrate catalyzed by supported heteropolyacid catalysts. Chinese Journal of Inorganic Chemistry, 2026, 42(3): 441-452. doi: 10.11862/CJIC.20250303
10. [10]
  Yongwei ZHANG , Chuang ZHU , Wenbin WU , Yongyong MA , Heng YANG . Efficient hydrogen evolution reaction activity induced by ZnSe@nitrogen doped porous carbon heterojunction. Chinese Journal of Inorganic Chemistry, 2025, 41(4): 650-660. doi: 10.11862/CJIC.20240386
11. [11]
  Sumiya Akter Dristy , Md Ahasan Habib , Shusen Lin , Mehedi Hasan Joni , Rutuja Mandavkar , Young-Uk Chung , Md Najibullah , Jihoon Lee . Exploring Zn doped NiBP microspheres as efficient and stable electrocatalyst for industrial-scale water splitting. Acta Physico-Chimica Sinica, 2025, 41(7): 100079-0. doi: 10.1016/j.actphy.2025.100079
12. [12]
  Lingling Li , Zhe Chen . Charge transfer mechanism investigation of S-scheme photocatalyst using soft X-ray absorption spectroscopy. Acta Physico-Chimica Sinica, 2026, 42(4): 100215-0. doi: 10.1016/j.actphy.2025.100215
13. [13]
  Zhanggui DUAN , Yi PEI , Shanshan ZHENG , Zhaoyang WANG , Yongguang WANG , Junjie WANG , Yang HU , Chunxin LÜ , Wei ZHONG . Preparation of UiO-66-NH₂ supported copper catalyst and its catalytic activity on alcohol oxidation. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 496-506. doi: 10.11862/CJIC.20230317
14. [14]
  Qinhui Guan , Yuhao Guo , Na Li , Jing Li , Tingjiang Yan . Molecular sieve-mediated indium oxide catalysts for enhancing photocatalytic CO₂ hydrogenation. Acta Physico-Chimica Sinica, 2025, 41(11): 100133-0. doi: 10.1016/j.actphy.2025.100133
15. [15]
  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
16. [16]
  Kun WANG , Wenrui LIU , Peng JIANG , Yuhang SONG , Lihua CHEN , Zhao DENG . Hierarchical hollow structured BiOBr-Pt catalysts for photocatalytic CO₂ reduction. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1270-1278. doi: 10.11862/CJIC.20240037
17. [17]
  Xueting Feng , Ziang Shang , Rong Qin , Yunhu Han . Advances in Single-Atom Catalysts for Electrocatalytic CO₂ Reduction. Acta Physico-Chimica Sinica, 2024, 40(4): 2305005-0. doi: 10.3866/PKU.WHXB202305005
18. [18]
  Qing Li , Guangxun Zhang , Yuxia Xu , Yangyang Sun , Huan Pang . P-Regulated Hierarchical Structure Ni₂P Assemblies toward Efficient Electrochemical Urea Oxidation. Acta Physico-Chimica Sinica, 2024, 40(9): 2308045-0. doi: 10.3866/PKU.WHXB202308045
19. [19]
  Jiali Lei , Juan Wang , Wenhui Zhang , Guohong Wang , Zihui Liang , Jinmao Li . TiO₂/CdIn₂S₄ S-scheme heterojunction photocatalyst promotes photocatalytic hydrogen evolution coupled vanillyl alcohol oxidation. Acta Physico-Chimica Sinica, 2025, 41(12): 100174-0. doi: 10.1016/j.actphy.2025.100174
20. [20]
  Qingqing SHEN , Xiangbowen DU , Kaicheng QIAN , Zhikang JIN , Zheng FANG , Tong WEI , Renhong LI . Self-supporting Cu/α-FeOOH/foam nickel composite catalyst for efficient hydrogen production by coupling methanol oxidation and water electrolysis. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1953-1964. doi: 10.11862/CJIC.20240028

Get Citation

PDF

XML

Metrics

PDF Downloads(23)
Abstract views(7687)
HTML views(1249)

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