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Evaluation of the physiochemical properties and catalytic performance of CuCoMnAl mixed oxides derived from layered double hydroxides precursors with different mole ratios of Cu/Co on the oxidation of toluene

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Abstract

CuCoMnAl mixed oxides with different mole ratios of Cu/Co were synthesized by thermal decomposition of layered double hydroxides (LDHs) precursors. They were characterized using X-ray diffraction, scanning electron microscopy, N2 adsorption/desorption isotherm analysis, H2-temperature program reduction and X-ray photoelectron spectroscopy, and their catalytic properties were evaluated in the total oxidation of toluene. The precursors of LDHs consisted in hydrotalcite phase with gerhardtite, malachite and rhodochrosite phase for Cu-containing systems. The mixed metal oxide derived from LDHs contains tenorite phases and different spinel (Co3O4, CoAl2O4 and Co2AlO4) phases. XPS analysis confirmed the existence of copper, cobalt and manganese with different valence states in the Cu, Co, Mn-containing mixed oxides. H2-TPR analysis indicated that the reduction peaks of cobalt and manganese were significantly shifted to lower temperatures for Cu–Co–Mn–Al samples by doping a small amount of Cu. BET analysis showed the increase of large mesopores and macropores of the samples with the increase of Cu contents. Cu2Co2MnAl-MMO present the best catalytic activity at all temperature range. The synergetic interactions among Co, Cu and Mn species, Mn3+ and lattice oxygen were beneficial for the best catalytic activity of Cu2Co2MnAl-MMO.

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References

  1. Liotta LF (2010) Catalytic oxidation of volatile organic compounds on supported noble metals. Appl Catal B 100:403–412

    CAS  Google Scholar 

  2. Li WB, Wang JX, Gong H (2009) Catalytic combustion of VOCs on non-noble metal catalysts. Catal Today 148:81–87

    CAS  Google Scholar 

  3. Hansen AB, Palmgren F (1996) VOC air pollutants in Copenhagen. Sci Total Environ 189:451–457

    Google Scholar 

  4. Atkinson R (2000) Atmospheric chemistry of VOCs and NOx. Atmos Environ 34:2063–2101

    CAS  Google Scholar 

  5. Amann M, Lutz M (2000) The revision of the air quality legislation in the European Union related to ground-level ozone. J Hazard Mater 78:41–62

    CAS  PubMed  Google Scholar 

  6. Fenske JD, Paulson SE (1999) Human breath emissions of VOCs. J Air Waste Manage 49:594–598

    CAS  Google Scholar 

  7. Everaert K, Baeyens J (2004) Catalytic combustion of volatile organic compounds. J Hazard Mater 109:113–139

    CAS  PubMed  Google Scholar 

  8. Gennequin C, Siffert S, Cousin R, Aboukaïs A (2009) Co-Mg-Al hydrotalcite precursors for catalytic total oxidation of volatile organic compounds. Top Catal 52:482–491

    CAS  Google Scholar 

  9. Sang CK, Wang GS (2010) Catalytic combustion of VOCs over a series of manganese oxide catalysts. Appl Catal B 98:180–185

    Google Scholar 

  10. Pinard L, Mijoin J, Magnoux P, Guisnet M (2003) Oxidation of chlorinated hydrocarbons over Pt zeolite catalysts 1-mechanism of dichloromethane transformation over PtNaY catalysts. J Catal 215:234–244

    CAS  Google Scholar 

  11. Stoylkova T, Chanev C (2016) Aerial oxidation of alcohols over CuAl-, CoAl-, NiAl-, ZnAl- layered double hydroxides and their mixed oxides. Reac Kinet Mech Cat 117:47–58

    CAS  Google Scholar 

  12. Zazhigalov S, Elyshev A, Lopatin S, Larina T, Cherepanova S, Mikenin P, Pisarev D, Baranov D, Zagoruiko A (2017) Copper-chromite glass fiber catalyst and its performance in the test reaction of deep oxidation of toluene in air. Reac Kinet Mech Cat 120:247–260

    CAS  Google Scholar 

  13. Wang L, Yin G, Yang Y, Zhang X (2019) Enhanced CO oxidation and toluene oxidation on CuCeZr catalysts derived from UiO-66 metal organic frameworks. Reac Kinet Mech Cat. https://doi.org/10.1007/s11144-019-01623-8

    Article  Google Scholar 

  14. Liotta LF, Ousmane M, Carlo GD, Pantaleo G, Deganello G, Boreave A, Giroir-Fendler A (2009) Catalytic removal of toluene over Co3O4–CeO2 mixed oxide catalysts: comparison with Pt/Al2O3. Catal Lett 127:270–276

    CAS  Google Scholar 

  15. He S, An Z, Wei M, Evans DG, Duan X (2013) Layered double hydroxide-based catalysts: nanostructure design and catalytic performance. Chem Commun 49:5912–5920

    CAS  Google Scholar 

  16. Huang ZJ, Wu PX, Gong BN, Fang Y, Zhu NW (2015) Fabrication and photocatalytic properties of a visible-light responsive nanohybrid based on self-assembly of carboxyl graphene and ZnAl layered double hydroxides. J Mater Chem A 2:5534–5540

    Google Scholar 

  17. Sideris PJ, Nielsen UG, Gan Z, Grey CP (2008) Mg/Al ordering in layered double hydroxides revealed by multinuclear NMR spectroscopy. Science 321:113–117

    CAS  PubMed  Google Scholar 

  18. Jirátová K, Mikulová J, Klempa J, Grygar T, Bastl Z, Kovanda F (2009) Modification of Co-Mn-Al mixed oxide with potassium and its effect on deep oxidation of VOC. Appl Catal A 361:106–116

    Google Scholar 

  19. Lamonier JF, Boutound AB, Gennequin C, Pérez-Zurita MJ, Siffert S, Aboukais A (2007) Catalytic removal of toluene in air over Co-Mn-Al nano-oxides synthesized by hydrotalcite route. Catal Lett 118:165–172

    CAS  Google Scholar 

  20. Obalová L, Maniak G, Karásková K, Kovanda F, Kotarba A (2011) Electronic nature of potassium promotion effect in Co-Mn-Al mixed oxide on the catalytic decomposition of N2O. Catal Commun 12:1055–1058

    Google Scholar 

  21. Kovanda F, Jirátová R, Ryměs J, Koloŭsek D (2001) Characterization of activated Cu/Mg/Al hydrotalcites and their catalytic activity in toluene combustion. Appl Clay Sci 18:71–80

    Google Scholar 

  22. Li S, Wang H, Li W, Wu X, Tang W, Chen Y (2015) Effect of Cu substitution on promoted benzene oxidation over porous CuCo-based catalysts derived from layered double hydroxide with resistance of water vapor. Appl Catal B 166–167:260–269

    Google Scholar 

  23. Li D, Fan Y, Ding Y, Wei X, Xiao Y (2017) Preparation of cobalt-copper-aluminum spinel mixed oxides from layered double hydroxides for total oxidation of benzene. Catal Commun 88:60–63

    Google Scholar 

  24. Li W, Wu PX, Zhu YJ, Huang ZJ, Lu YH, Li YW, Dang Z, Zhu NW (2015) Catalytic degradation of bisphenol A by CoMnAl mixed metal oxides catalyzed peroxymonosulfate. Chem Eng J 279:93–102

    CAS  Google Scholar 

  25. Kanezaki E (1998) Direct observation of a metastable solid phase of Mg/Al/CO3-layered double hydroxide by means of high temperature in situ powder XRD and DTA/TG. Inorg Chem 37:2588–2590

    CAS  Google Scholar 

  26. Stanimirova TS, Vergilov I, Kirov G, Petrova N (1999) Thermal decomposition products of hydrotalcite-like compounds: low-temperature metaphases. J Mater Sci 34:4153–4161

    CAS  Google Scholar 

  27. Kosova NV, Devyatkina ET, Kaichev VV (2007) Mixed layered Ni-Mn-Co hydroxides: crystal structure, electronic state of ions, and thermal decomposition. J Power Sources 174:735–740

    CAS  Google Scholar 

  28. Yamaoka T, Abe M, Tsuji M (1989) Synthesis of Cu-Al hydrotalcite like compound and its ion exchange property. Mater Res Bull 24:1183–1199

    CAS  Google Scholar 

  29. Zhang Y, Qin Z, Wang G, Zhu H, Dong M, Li S, Wu Z, Li Z, Wu Z, Zhang J, Hu T, Fan W, Wang J (2013) Catalytic performance of MnOx–NiO composite oxide in lean methane combustion at low temperature. Appl Catal B 129:172

    CAS  Google Scholar 

  30. Li H, Lu G, Dai Q, Wang Y, Guo Y, Guo Y (2011) Efficient low-temperature catalytic combustion of trichloroethylene over flower-like mesoporous Mn-doped CeO2 microspheres. Appl Catal B 102:475–483

    CAS  Google Scholar 

  31. Pérez H, Navarro P, Delgado JJ, Montes M (2011) Mn-SBA15 catalysts prepared by impregnation: influence of the manganese precursor. Appl Catal A 400:38–248

    Google Scholar 

  32. Deng L, Ding Y, Duan B, Chen Y, Li P, Zhu S, Shen S (2018) Catalytic deep combustion characteristics of benzene over cobalt doped Mn-Ce solid solution catalysts at lower temperatures. Mol Catal 446:72–80

    CAS  Google Scholar 

  33. Gao W, Zhao Y, Liu J, Huang Q, He S, Li C, Zhao J, Wei M (2013) Catalytic conversion of syngas to mixed alcohols over CuFe-based catalysts derived from layered double hydroxides. Catal Sci Technol 3:1324–1332

    CAS  Google Scholar 

  34. Papavasiliou J, Avgouropoulos G, Ioannides T (2007) Combined steam reforming of methanol over Cu–Mn spinel oxide catalysts. J Catal 251:7–20

    CAS  Google Scholar 

  35. Elp JV, Weiland JL, Eskes H, Kuiper P, Sawatzky GA, Degroot FMF, Turner T (1991) Electronic structure of CoO, Li-doped CoO, and LiCoO2. Phys Rev B 44:6090–6103

    Google Scholar 

  36. Degroot FMF, Abbate M, Elp JV, Sawatzky GA, Ma YJ, Chen CT, Sette F (1993) Oxygen 1s and cobalt 2p X-ray absorption of cobalt oxides. J Phys-Condens Matter 5:2277–2288

    CAS  Google Scholar 

  37. Mizokawa T, Tjeng LH, Steeneken PG, Brookes NB, Tsukada I, Yamamoto T, Uchinokura K (2001) Photoemission and X-ray-adsorption study of misfit-layered (Bi, Pb)-Sr-Co-O compounds: electronic structure of a hole-doped Co-O triangular lattice. Phys Rev B 64:115104

    Google Scholar 

  38. McFarland EW, Metiu H (2013) Catalysis by doped oxides. Chem Rev 113:4391–4427

    CAS  PubMed  Google Scholar 

  39. Wang Z, Shen G, Li J, Liu H, Wang Q, Chen Y (2013) Catalytic removal of benzene over CeO2-MnOx composite oxides prepared by hydrothermal method. Appl Catal B 138–139:253–259

    Google Scholar 

  40. Ribet S, Tichit D, Coq B, Ducourant B, Morato F (1999) Synthesis and activation of Co–Mg–Al layered double hydroxides. J Solid State Chem 142:382–392

    CAS  Google Scholar 

  41. Arnoldy P, Moulijn JA (1985) Temperature-programmed reduction of CoOAl2O3 catalysts. J Catal 93:38–54

    CAS  Google Scholar 

  42. Sexton BA, Hughes AE, Turney TW (1986) An XPS and TPR study of the reduction of promoted cobalt-kieselguhr Fischer-Tropsch catalysts. J Catal 97:390–406

    CAS  Google Scholar 

  43. Morales MR, Barbero BP, Cadús LE (2008) Evaluation and characterization of Mn-Cu mixed oxide catalysts for ethanol total oxidation: influence of copper content. Fuel 87:1177–1186

    CAS  Google Scholar 

  44. Velu S, Suzuki K, Hashimoto S, Satoh N, Ohashia F, Tomura S (2001) The effect of cobalt on the structural properties and reducibility of CuCoZnAl layered double hydroxides and their thermally derived mixed oxides. J Mater Chem 11:2049–2060

    CAS  Google Scholar 

Download references

Acknowledgements

This research described above was supported by the Key Platform and Major Scientific Research Project from Education Department of Guangdong Province (Grant No. 2017GKTSCX037), Presidential Foundation of Guangdong Polytechnic of Environmental Protection Engineering (Grant No. K640118122012) and National Science Foundation of China (Grant No. 51508245).

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Authors and Affiliations

  1. Guangdong Polytechnic of Environmental Protection Engineering, Foshan, 528216, Guangdong, People’s Republic of China

    Wen Li, Keliang Wang & Shunheng Tu

  2. School of Environment and Energy, South China University of Technology, Guangzhou, 510006, People’s Republic of China

    Shanshan Yang & Pingxiao Wu

  3. School of Environmental and Land Resource Management, Jiangxi Agricultural University, Nanchang, 330045, People’s Republic of China

    Meijuan Lu

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  1. Wen Li
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Correspondence to Wen Li.

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Li, W., Yang, S., Wang, K. et al. Evaluation of the physiochemical properties and catalytic performance of CuCoMnAl mixed oxides derived from layered double hydroxides precursors with different mole ratios of Cu/Co on the oxidation of toluene. Reac Kinet Mech Cat 128, 965–977 (2019). https://doi.org/10.1007/s11144-019-01676-9

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