Abstract
In this study, pure phase Cu2.5Mn0.5MgAl precursor was synthesized by layered double hydroxides (LDHs) precursor template method. Subsequently, Cu2.5Mn0.5MgAl-LDH is calcined at 500, 600 and 700 ℃ to obtain the corresponding layered double oxides (LDO) catalysts for simultaneous removal of NOx and toluene. The results show that Cu2.5Mn0.5MgAl-500 exhibits the best catalytic performance in both NOx reduction and toluene oxidation reactions and the conversion of NOx and toluene can reach 85% and 88% at 210 ℃, respectively. XRD, SEM, BET, NH3-TPD, H2-TPR, XPS and in situ DRIFT were applied to characterize the prepared catalysts. The obtained Cu2.5Mn0.5MgAl-500 has abundant acid sites, excellent redox capacity and the highest concentration of surface Mn4+ and Cu+ species, which are considered to be the main factors determining its excellent catalytic performance. In addition, Cu2.5Mn0.5MgAl-500 shows superior durability and good tolerance to H2O/SO2.
Graphical Abstract
Similar content being viewed by others
References
Sun L, Cao Q, Hu B, Li J, Hao J, Jing G, Tang X (2011) Synthesis, characterization and catalytic activities of vanadium–cryptomelane manganese oxides in low-temperature NO reduction with NH3. Appl Catal A Gen 393:323–330
Yan X, Anguille S, Bendahan M, Moulin P (2021) Toluene removal from gas streams by an ionic liquid membrane: experiment and modeling. Chem Eng J 404:127109
Luo Y, Zheng Y, Zuo J, Feng X, Wang X, Zhang T, Zhang K, Jiang L (2018) Insights into the high performance of Mn-Co oxides derived from metal-organic frameworks for total toluene oxidation. J Hazard Mater 349:119–127
Feng Z, Ren Q, Peng R, Mo S, Zhang M, Fu M, Chen L, Ye D (2019) Effect of CeO2 morphologies on toluene catalytic combustion. Catal Today 332:177–182
Zhao S, Li K, Jiang S, Li J (2016) Pd–Co based spinel oxides derived from pd nanoparticles immobilized on layered double hydroxides for toluene combustion. Appl Catal B Environ 181:236–248
Li X, Li K, Peng Y, Li X, Zhang Y, Wang D, Chen J, Li J (2018) Interaction of phosphorus with a FeTiOx catalyst for selective catalytic reduction of NOx with NH3: Influence on surface acidity and SCR mechanism. Chem Eng J 347:173–183
Guo Y, Wen M, Li G, An T (2021) Recent advances in VOC elimination by catalytic oxidation technology onto various nanoparticles catalysts: a critical review. Appl Catal B Environ 281:119447
Zhang Y, Xiong Z, Yang Q, Zhou F, Lu W, Shi H (2022) Influence of copper doping on the low-medium NH3-SCR activity of magnetic W/Fe2O3 catalyst: its synergetic effect of glucose dosage. J Environ Chem Eng 10:108694
Deng W, Tang Q, Huang S, Zhang L, Jia Z, Guo L (2020) Low temperature catalytic combustion of chlorobenzene over cobalt based mixed oxides derived from layered double hydroxides. Appl Catal B Environ 278:119336
Zhao L, Huang Y, Zhang J, Jiang L, Wang Y (2020) Al2O3-modified CuO-CeO2 catalyst for simultaneous removal of NO and toluene at wide temperature range. Chem Eng J 397:125419
Yan Q, Nie Y, Yang R, Cui Y, O’Hare D, Wang Q (2017) Highly dispersed CuyAlOx mixed oxides as superior low-temperature alkali metal and SO2 resistant NH3-SCR catalysts. Appl Catal A Gen 538:37–50
Wu X, Meng H, Du Y, Liu J, Hou B, Xie X (2019) Fabrication of highly dispersed Cu-based oxides as desirable NH3-SCR catalysts via employing CNTs to decorate the CuAl-layered double hydroxides. ACS Appl Mater Inter 11:32917–32927
Kovanda F (2001) Characterization of activated Cu/Mg/Al hydrotalcites and their catalytic activity in toluene combustion. Appl Clay Sci 18:71–80
Xu G, Guo X, Cheng X, Yu J, Fang B (2021) A review of Mn-based catalysts for low-temperature NH3-SCR: NOx removal and H2O/SO2 resistance. Nanoscale 13:7052–7080
Kim SC, Shim WG (2010) Catalytic combustion of VOCs over a series of manganese oxide catalysts. Appl Catal B Environ 98:180–185
Yan Q, Chen S, Qiu L, Gao Y, O’Hare D, Wang Q (2018) The synthesis of CuyMnzAl1-zOx mixed oxide as a low-temperature NH3-SCR catalyst with enhanced catalytic performance. Dalton T 47:2992–3004
Aguilera DA, Perez A, Molina R, Moreno S (2011) Cu–Mn and Co–Mn catalysts synthesized from hydrotalcites and their use in the oxidation of VOCs. Appl Catal B Environ 104:144–150
Mo S, Li S, Li W, Li J, Chen J, Chen Y (2016) Excellent low temperature performance for total benzene oxidation over mesoporous CoMnAl composited oxides from hydrotalcites. J Mater Chem A 4:8113–8122
Xue T, Li R, Zhang Z, Gao Y, Wang Q (2020) Preparation of MnO2 decorated Co3Fe1Ox powder/monolithic catalyst with improved catalytic activity for toluene oxidation. J Environ Sci 96:194–203
Wu X, Liu J, Liu X, Wu X, Du Y (2022) Fabrication of carbon doped Cu-based oxides as superior NH3-SCR catalysts via employing sodium dodecyl sulfonate intercalating CuMgAl-LDH. J Catal 407:265–280
Chakraborty S, Kumar M, Suresh K, Pugazhenthi G (2014) Influence of organically modified NiAl layered double hydroxide (LDH) loading on the rheological properties of poly (methyl methacrylate) (PMMA)/LDH blend solution. Powder Technol 256:196–203
Wang R, Wu X, Zou C, Li X, Du Y (2018) NOx removal by selective catalytic reduction with ammonia over a hydrotalcite-derived NiFe mixed oxide. Catal 8:384
Li H, Zhu G, Yang Z, Wang Z, Liu ZH (2010) Preparation and capacitance property of MnO2-pillared Ni2+-Fe3+ layered double hydroxides nanocomposite. J Colloid Interf Sci 345:228–233
Chen L, Li R, Li Z, Yuan F, Niu X, Zhu Y (2017) Effect of Ni doping in NixMn1−xTi10 (x = 0.1–0.5) on activity and SO2 resistance for NH3-SCR of NO studied with in situ DRIFTS. Catal Sci Technol 7:3243–3257
Hou B, Du Y, Liu X, Ci C, Wu X, Xie X (2019) Tunable preparation of highly dispersed NixMn-LDO catalysts derived from NixMn-LDHs precursors and application in low-temperature NH3-SCR reactions. RSC Adv 9:24377–24385
Du Y, Liu J, Li X, Liu L, Wu X (2020) SCR performance enhancement of NiMnTi mixed oxides catalysts by regulating assembling methods of LDHs-Based precursor. Appl Organomet Chem 34:e5510
Wu X, Feng Y, Du Y, Liu X, Zou C, Li Z (2019) Enhancing DeNOx performance of CoMnAl mixed metal oxides in low-temperature NH3-SCR by optimizing layered double hydroxides (LDHs) precursor template. Appl Surf Sci 467:802–810
Tang W, Wu X, Li S, Shan X, Liu G, Chen Y (2015) Co-nanocasting synthesis of mesoporous Cu–Mn composite oxides and their promoted catalytic activities for gaseous benzene removal. Appl Catal B Environ 162:110–121
Gélin P, Primet M (2002) Complete oxidation of methane at low temperature over noble metal based catalysts: a review. Appl Catal B Environ 39:1–37
Gawande MB, Goswami A, Felpin FX, Asefa T, Huang X, Silva R, Zou X, Zboril R, Varma RS (2016) Cu and Cu-based nanoparticles: synthesis and applications in catalysis. Chem Rev 116:3722–3811
Yang Y, Yan X, Hu X, Feng R, Zhou M, Cui W (2018) Development of zeolitic imidazolate framework-67 functionalized Co-Al LDH for CO2 adsorption. Colloids Surface A 552:16–23
Zhao K, Meng J, Lu J, He Y, Huang H, Tang Z, Zhen X (2018) Sol-gel one-pot synthesis of efficient and environmentally friendly iron-based catalysts for NH3-SCR. Appl Surf Sci 445:454–461
Fang C, Zhang D, Cai S, Zhang L, Huang L, Li H, Maitarad P, Shi L, Gao R, Zhang J (2013) Low-temperature selective catalytic reduction of NO with NH3 over nanoflaky MnOx on carbon nanotubes in situ prepared via a chemical bath deposition route. Nanoscale 5:9199–9207
Xiong S, Huang N, Peng Y, Chen J, Li J (2021) Balance of activation and ring-breaking for toluene oxidation over CuO-MnOx bimetallic oxides. J Hazard Mater 415:125637
Chen Z, Fan C, Pang L, Ming S, Liu P, Zhu D, Wang J, Cai X, Chen H, Lai Y, Li T (2018) Direct synthesis of submicron Cu-SAPO-34 as highly efficient and robust catalyst for selective catalytic reduction of NO by NH3. Appl Surf Sci 448:671–680
KaráskováK ObalováL, Jirátová K, Kovanda F (2010) Effect of promoters in Co–Mn–Al mixed oxide catalyst on N2O decomposition. Chem Eng J 160:480–487
He Z, Lin H, He P, Yuan Y (2011) Effect of boric oxide doping on the stability and activity of a Cu–SiO2 catalyst for vapor-phase hydrogenation of dimethyl oxalate to ethylene glycol. J Catal 277:54–63
Tang X, Li J, Sun L, Hao J (2010) Origination of N2O from NO reduction by NH3 over β-MnO2 and α-Mn2O3. Appl Catal B Environ 99:156–162
Wu Y, Lu Y, Song C, Ma Z, Xing S, Gao Y (2013) A novel redox-precipitation method for the preparation of α-MnO2 with a high surface Mn4+ concentration and its activity toward complete catalytic oxidation of o-xylene. Catal Today 201:32–39
Chen S, Vasiliades M A, Yan Q, Yang G, Du X, Zhang C, Li Y, Zhu T, Wang Q, Efstathiou A M (2020) Remarkable N2-selectivity enhancement of practical NH3-SCR over Co0.5Mn1Fe0.25Al0.75Ox-LDO: The role of Co investigated by transient kinetic and DFT mechanistic studies. Appl Catal B Environ 277:119186
Gao C, Xiao B, Shi JW, He C, Wang B, Ma D, Cheng Y, Niu C (2019) Comprehensive understanding the promoting effect of Dy-doping on MnFeOx nanowires for the low-temperature NH3-SCR of NOx: an experimental and theoretical study. J Catal 380:55–67
Liu F, He H, Zhang C, Feng Z, Zheng L, Xie Y, Hu T (2010) Selective catalytic reduction of NO with NH3 over iron titanate catalyst: catalytic performance and characterization. Appl Catal B Environ 96:408–420
Li Q, Yang H, Qiu F, Zhang X (2011) Promotional effects of carbon nanotubes on V2O5/TiO2 for NOx removal. J Hazard Mater 192:915–921
Yu T, Hao T, Fan D, Wang J, Shen M, Li W (2014) Recent NH3-SCR mechanism research over Cu/SAPO-34 catalyst. J Phys Chem C 118:6565–6575
Wei Y, Fan H, Wang R (2018) Transition metals (Co, Zr, Ti) modified iron-samarium oxide as efficient catalysts for selective catalytic reduction of NOx at low-temperature. Appl Surf Sci 459:63–73
Wang Z, Lan J, Haneda M, Liu Z (2021) Selective catalytic reduction of NOx with NH3 over a novel Co-Ce-Ti catalyst. Catal Today 376:222–228
Yang W, Su ZA, Xu Z, Yang W, Peng Y, Li J (2020) Comparative study of α-, β-, γ- and δ-MnO2 on toluene oxidation: oxygen vacancies and reaction intermediates. Appl Catal B Environ 260:118150
Ye L, Lu P, Chen X, Fang P, Peng Y, Li J, Huang H (2020) The deactivation mechanism of toluene on MnOx-CeO2 SCR catalyst. Appl Catal B Environ 277:119257
Xu W, He H, Yu Y (2009) Deactivation of a Ce/TiO2 catalyst by SO2 in the selective catalytic reduction of NO by NH3. J Phys Chem C 113:4426–4432
Ma L, Seo CY, Chen X, Sun K, Schwank JW (2018) Indium-doped Co3O4 nanorods for catalytic oxidation of CO and C3H6 towards diesel exhaust. Appl Catal B Environ 222:44–58
Chen X, Chen X, Cai S, Yu E, Chen J, Jia H (2019) MnOx/Cr2O3 composites prepared by pyrolysis of Cr-MOF precursors containing in situ assembly of MnOx as high stable catalyst for toluene oxidation. Appl Surf Sci 475:312–324
Chen J, Chen X, Xu W, Xu Z, Chen J, Jia H, Chen J (2017) Hydrolysis driving redox reaction to synthesize Mn-Fe binary oxides as highly active catalysts for the removal of toluene. Chem Eng J 330:281–293
Sun H, Liu Z, Chen S, Quan X (2015) The role of lattice oxygen on the activity and selectivity of the OMS-2 catalyst for the total oxidation of toluene. Chem Eng J 270:58–65
Zhao Y, Zhao B, Zhuo Y, Chen C, Xu X (2012) A study of the mechanism of iron-based sulfate catalyst for selective catalytic reduction of NO with NH3. Asia Pac J Chem Eng 7:581–589
Long R, Yang R (2000) Characterization of Fe-ZSM-5 catalyst for selective catalytic reduction of nitric oxide by ammonia. J Catal 194:80–90
Zhang X, Ma ZA, Song Z, Zhao H, Liu W, Zhao M, Zhao J (2019) Role of cryptomelane in surface-adsorbed oxygen and Mn chemical valence in MnOx during the catalytic oxidation of toluene. J Phys Chem C 123:17255–17264
Li Z, Gao Y, Wang Q (2022) The influencing mechanism of NH3 and NOx addition on the catalytic oxidation of toluene over Mn2Cu1Al1Ox catalyst. J Clean Prod 348:131152
Acknowledgements
This work was supported by the National Natural Science Foundation of China (51978436, 22272116).
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Below is the link to the electronic supplementary material.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Wei, F., Liu, L., Wu, X. et al. Simultaneous Removal of NOx and Toluene on CuMnMgAl Layered Double Oxides (LDO) Derived from Layered Double Hydroxides (LDHs) Precursor. Catal Lett 154, 1184–1200 (2024). https://doi.org/10.1007/s10562-023-04384-1
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10562-023-04384-1