Abstract
A series of MnOx/ACFN, Ce-MnOx/ACFN, and Fe-Ce-MnOx/ACFN catalysts on selective catalytic reduction (SCR) of NOx with NH3 at low-middle temperature had been successfully prepared through ultrasonic impregnation method, and the catalysts were characterized by SEM, XRD, BET, H2-TPR, NH3-TPD, XPS, and FT-IR spectroscopy, respectively. The results demonstrated that the 15 wt% Fe(1)-Ce(3)-MnOx(7)/ACFN catalyst achieved 90% NOx conversion (100~300 °C), good water resistance, and stability (175 °C). The excellent catalytic performance of the Fe(1)-Ce(3)-MnOx(7)/ACFN catalyst was mainly attributed to the interaction among Mn, Ce, and Fe. The doping of Fe promoted the dispersion of Ce and Mn and the formation of more Mn4+ and chemisorbed oxygen on the surface of a catalyst. This work laid a foundation for the successful application of active carbon fiber in the field of industrial denitrification, especially in the aspect of denitrification moving bed.
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Anthonysamy SBI, Binti AS, Mehrnoush K, Mohamed ARB (2018) A review of carbon-based and non-carbon-based catalyst supports for the selective catalytic reduction of nitric oxide. Beilstein J. Nanotechnol 9:740–761. https://doi.org/10.3762/bjnano.9.68
Cao F, Xiang J, Su S, Wang PY, Sun LS, Hu S, Lei SY (2014) The activity and characterization of MnOx-CeO2-ZrO2/γ-Al2O3 catalysts for low temperature selective catalytic reduction of NO with NH3. Chem Eng J 243:347–354. https://doi.org/10.1016/j.apcatb.2013.10.049
Cao F, Su S, Xiang J, Wang PX, Hu S, Sun LS, Zhang AC (2015) The activity and mechanism study of Fe-Mn-Ce/γ-Al2O3 catalyst for low temperature selective catalytic reduction of NO with NH3. Fuel 139:232–239. https://doi.org/10.1016/j.fuel.2014.08.060
Chang HZ, Li JH, Chen XY, Ma L, Yang SJ, Schwank JW, Hao JM (2012) Effect of Sn on MnOx-CeO2 catalyst for SCR of NOx by ammonia: enhancement of activity and remarkable resistance to SO2. Catal Commun 27:54–57. https://doi.org/10.1016/j.catcom.2012.06.022
Chen QL, Guo RT, Wang QS, Pan WG, Wang WH, Yang NZ, Lu CZ, Wang SX (2016) The catalytic performance of Mn/TiWOx catalyst for selective catalytic reduction of NOx with NH3. Fuel 181:852–858. https://doi.org/10.1016/j.fuel.2016.05.045
Fan XY, Yang HS, Tian W, Nie AM, Hou TF, Qiu FM, Zhang XB (2011) Catalytic oxidation of chlorobenzene over MnOx/Al2O3-carbon nanotubes composites. Catal Letter 141(1):158–162. https://doi.org/10.1007/s10562-010-0450-9
Fan ZY, Shi JW, Gao C, Gao G, Wang BR, Wang Y, He C, Niu CM (2018) Gd-modified MnOx for the selective catalytic reduction of NO by NH3: the promoting effect of Gd on the catalytic performance and sulfur resistance. Chem Eng J 348:820–830. https://doi.org/10.1016/j.cej.2018.05.038
Fang NJ, Guo JX, Shu S, Luo HD, Chu YH, Li JJ (2017) Enhancement of low-temperature activity and sulfur resistance of Fe0.3Mn0.5Zr0.2 catalyst for NO removal by NH3-SCR. Chem Eng J 325:114–123. https://doi.org/10.1021/am5038164
France LJ, Yang Q, Li W, Chen ZH, Guang JY, Guo DW, Wang LF, Li XH (2017) Ceria modified FeMnOx-enhanced performance and sulphur resistance for low-temperature SCR of NOx. Appl Catal B Environ 206:203–215. https://doi.org/10.1016/j.apcatb.2017.01.019
Gao FY, Tang XL, Yi HH, Li JY, Zhao SZ, Wang JG, Chu C, Li CL (2017a) Promotional mechanisms of activity and SO2 tolerance of Co- or Ni-doped MnOx-CeO2 catalysts for SCR of NOx with NH3 at low temperature. Chem Eng J 317:20–31. https://doi.org/10.1016/j.cej.2017.02.042
Gao FY, Tang XL, Yi HH, Zhao SZ, Li CL, Li JY, Shi YR, Meng XM (2017b) A review on selective catalytic reduction of NOx by NH3 over Mn-based catalysts at low temperatures: catalysts, mechanisms, kinetics and DFT calculations. Catalysts 7(7):199. https://doi.org/10.3390/catal7070199
Gao FY, Tang XL, Yi HH, Zhao SZ, Wang JG, Gu T (2019) Improvement of activity, selectivity and H2O&SO2-tolerance of micro-mesoporous CrMn2O4 spinel catalyst for low-temperature NH3-SCR of NOx. Appl Surf Sci 466:411–424. https://doi.org/10.1016/j.apsusc.2018.09.227
Grzybek T, Klinik J, Motak M, Papp H (2008) Nitrogen-promoted active carbons as catalytic supports. Catal Today 137(2-4):235–241. https://doi.org/10.1016/j.cattod.2007.11.006
Hu G, Yang J, Tian YM, Kong BW, Liu QC, Ren S, Li JL, Kong M (2018) Effect of Ce doping on the resistance of Na over V2O5-WO3/TiO2 SCR catalysts. Mater Res Bull 104:112–118. https://doi.org/10.1016/j.materresbull.2018.04.009
Huang HC, Ye DQ, Huang BC, Wei ZL (2008) Vanadium supported on viscose-based activated carbon fibers modified by oxygen plasma for the SCR of NO. Catal Today 139(1-2):100–108. https://doi.org/10.1016/j.cattod.2008.08.028
Jiang LJ, Liu QC, Zhao Q, Ren S, Kong M, Yao L, Meng F (2018) Promotional effect of Ce on the SCR of NO with NH3 at low temperature over MnOx supported by nitric acid-modified activated carbon. Res Chem Intermed 44(3):1729–1744. https://doi.org/10.1007/s11164-017-3194-y
Li P, Lu P, Zhai Y, Li C, Chen T, Qing R, Zhang W (2015a) Low temperature SCR of NO with catalysts prepared by modified ACF loading Mn and Ce: effects of modification method. Environ Technol 36(18):2390–2400. https://doi.org/10.1080/09593330.2015.1031829
Li J, Yang CW, Zhang QQ, Li Z, Huang W (2015b) Effects of Fe addition on the structure and catalytic performance of mesoporous Mn/Al-SBA-15 catalysts for the reduction of NO with ammonia. Catal Commun 62:24–28. https://doi.org/10.1016/j.catcom.2015.01.003
Li YL, Han XJ, Hou YQ, Guo YP, Liu YJ, Cui Y, Huang ZG (2018a) Role of CTAB in the improved H2O resistance for selective catalytic reduction of NO with NH3 over iron titanium catalyst. Chem Eng J 347:313–321. https://doi.org/10.1016/j.cej.2018.04.107
Li G, Wang BD, Wang ZC, Li ZH, Sun Q, Xu WQ, Li YL (2018b) Reaction mechanism of low-temperature selective catalytic reduction of NOx over Fe-Mn oxides supported on fly-ash-derived SBA-15 molecular sieves: structure-activity relationships and in situ DRIFT analysis. J Phys Chem C 122(35):20210–20231. https://doi.org/10.1021/acs.jpcc.8b03135
Liu ZM, Yi Y, Zhang SX, Zhu TL, Zhu JZ, Wang JG (2013) Selective catalytic reduction of NOx with NH3 over Mn-Ce mixed oxide catalyst at low temperatures. Catal Today 216:76–81. https://doi.org/10.1016/j.cattod.2013.06.009
Liu ZM, Zhu JZ, Li JH, Ma L, Woo SI (2014) Novel Mn-Ce-Ti mixed-oxide catalyst for the selective catalytic reduction of NOx with NH3. Acs Appl Mater Inter 6:14500–14508. https://doi.org/10.1021/am5038164
Liu ZM, Feng X, Zhou ZZ, Feng YJ, Li JH (2018a) Ce-Sn binary oxide catalyst for the selective catalytic reduction of NOx by NH3. Appl Surf Sci 428:526–533. https://doi.org/10.1016/j.apsusc.2017.09.175
Liu ZM, Liu HY, Feng X, Ma LL, Cao XZ, Wang BY (2018b) Ni-Ce-Ti as a superior catalyst for the selective catalytic reduction of NOx with NH3. Mol Catal 445:179–186. https://doi.org/10.1016/j.mcat.2017.11.028
Lu P, Li CT, Zeng GM, He LJ, Peng DL, Cui HF, Li SH, Zhai YB (2010) Low temperature selective catalytic reduction of NO by activated carbon fiber loading lanthanum oxide and ceria. Appl Catal B-Environ 96:157–161. https://doi.org/10.1016/j.apcatb.2010.02.014
Lu XL, Zou HQ, Zhang YB, Qiu HF, Zheng YY (2015) Low-temperature selective catalytic reduction of NO over carbon nanotubes supported MnO2 fabricated by co-precipitation method. Micro Nano Lett 10(11):666–669. https://doi.org/10.1515/pac-2014-1117
Lu P, Xing Y, Li CT, Qing RP, Su W, Liu NA (2016) A reusable material with high performance for removing NO at room temperature: performance, mechanism and kinetics. Catal Sci Technol 6(10):3520–3528. https://doi.org/10.1039/c5cy01562f
Lu P, Li R, Xing Y, Li YR, Zhu TY, Yue HF, Wu WR (2018) Low temperature selective catalytic reduction of NOx with NH3 by activated coke loaded with FexCoyCezOm: the enhanced activity, mechanism and kinetics. Fuel 233:88–199. https://doi.org/10.1016/j.cej.2017.02.148
Ma L, Seo CY, Nahata M, Chen XY, Li JH, Schwank JW (2018) Shape dependence and sulfate promotion of CeO2 for selective catalytic reduction of NOx with NH3. Appl Catal B Environ 232:246–259. https://doi.org/10.1016/j.apcatb.2018.03.065
Marani D, Silva RH, Dankeaw A, Norrman K, Werchmeister RML, Ippolito D, Gudik-Sørensen M, Hansen KK, Esposito V (2017) NOx selective catalytic reduction (SCR) on self-supported V-W-doped TiO2 nanofibers. New J Chem 41(9):3466–3472. https://doi.org/10.1039/C6NJ03205B
Marbán G, Antu AR, Fuertes AB (2003) Low-temperature SCR of NOx with NH3 over activated carbon fiber composite-supported metal oxides. Appl Catal B Environ 41(3):323–338. https://doi.org/10.1016/S0926-3373(02)00170-4
Meng DM, Xu Q, Jiao YL, Guo Y, Guo Y, Wang L, Lu GZ, Zhan WC (2018) Spinel structured CoaMnbOx mixed oxide catalyst for the selective catalytic reduction of NOx with NH3. Appl Catal B Environ 221:652–663. https://doi.org/10.1016/j.apcatb.2017.09.034
Ramesh K, Chen LW, Chen FX, Liu Y, Wang Z, Han YF (2008) Re-investigating the CO oxidation mechanism over unsupported MnO, Mn2O3 and MnO2 catalysts. Catal Today 131(1-4):477–482. https://doi.org/10.1016/j.cattod.2007.10.061
Shen BX, Liu T, Shi ZL, Shi JW, Yang TT, Zhao N (2008) Low-temperature selective catalytic reduction of NO with NH3 based on MnOx-CeOx/ACFN. Front Chem Eng China 2(3):325–329. https://doi.org/10.1007/s11705-008-0053-9
Shen Q, Zhang LY, Sun NN, Wang H, Zhong LS, He C, Wei W, Sun YH (2017) Hollow MnOx-CeO2 mixed oxides as highly efficient catalysts in NO oxidation. Chem Eng J 322:46–55. https://doi.org/10.1016/j.cej.2017.02.148
Shen BX, Zhu SW, Zhang X, Chi GL, Patel D, Si M, Wu CF (2018) Simultaneous removal of NO and Hg0 using Fe and Co co-doped Mn-Ce/TiO2 catalysts. Fuel 224:241–249. https://doi.org/10.1016/j.fuel.2018.03.080
Sun X, Guo RT, Liu SW, Liu J, Pan WG, Shi X, Qin H, Wang ZY, Qiu ZZ, Liu XY (2018a) The promoted performance of CeO2 catalyst for NH3-SCR reaction by NH3 treatment. Appl Surf Sci 462:187–193. https://doi.org/10.1016/j.apsusc.2018.08.114
Sun P, Huang SX, Guo RT, Li MY, Liu SM, Pan WG, Fu ZG, Liu SW, Sun X, Liu J (2018b) The enhanced SCR performance and SO2 resistance of Mn/TiO2 catalyst by the modification with Nb: a mechanistic study. Appl Surf Sci 447:479–488. https://doi.org/10.1016/j.apsusc.2018.03.245
Sun CZ, Liu H, Chen W, Chen DZ, Yu SH, Liu AN, Dong L, Feng S (2018c) Insights into the Sm/Zr co-doping effects on N2 selectivity and SO2 resistance of a MnOx-TiO2 catalyst for the NH3-SCR reaction. Chem Eng J 347:27–40. https://doi.org/10.1016/j.cej.2018.04.029
Tang AD, Hu LQ, Yang XH, Jia YR, Zhang Y (2016) Promoting effect of the addition of Ce and Fe on manganese oxide catalyst for 1,2-dichlorobenzene catalytic combustion. Catal Commun 82:41–45. https://doi.org/10.1016/j.catcom.2016.04.015
Tang XL, Li CL, Yi HH, Wang LF, Yu QJ, Gao FY, Cui XX, Chu C, Li JY, Zhang RC (2018) Facile and fast synthesis of novel Mn2CoO4@rGO catalysts for the NH3-SCR of NOx at low temperature. Chem Eng J 333:467–476. https://doi.org/10.1016/j.cej.2017.09.179
Thommes M, Kaneko K, Neimark AV, Olivier JP, Rodriguez-Reinoso F, Rouquerol J, Sing KS (2015) (2015) Physisorption of gases, with special reference to the evaluation of surface area and pore size distribution (IUPAC technical report). Pure Appl. Chem. 87(9-10):1051–1069. https://doi.org/10.1515/pac-2014-1117
Tian W, Yang HS, Fan XY, Zhang XB (2011) Catalytic reduction of NOx with NH3 over different-shaped MnO2 at low temperature. J Hazard Mater 188(1-3):105–109. https://doi.org/10.1016/j.jhazmat.2011.01.078
Wan YP, Zhao WR, Tang Y, Li L, Wang HJ, Cui YL, Gu JL, Li YS, Shi JL (2014) Ni-Mn bi-metal oxide catalysts for the low temperature SCR removal of NO with NH3. Appl Catal B Environ 148-149:114–122. https://doi.org/10.1016/j.apcatb.2013.10.049
Wang YL, Ge CZ, Zhan L, Li C, Qiao WM, Ling LC (2012) MnOx-CeO2/activated carbon honeycomb catalyst for selective catalytic reduction of NO with NH3 at low temperatures. Ind Eng Chem Res 51(36):11667–11673. https://doi.org/10.1021/ie300555f
Wang MX, Liu HN, Huang ZH, Kang FY (2014) Activated carbon fibers loaded with MnO2 for removing NO at room temperature. Chem Eng J 256:101–106. https://doi.org/10.1016/j.cej.2014.06.108
Wang WT, Herreros JM, Tsolakis A, York APE (2015) Increased NO2 concentration in the diesel engine exhaust for improved Ag/Al2O3 catalyst NH3-SCR activity. Chem Eng J 270:582–589. https://doi.org/10.1016/j.cej.2015.02.067
Wang DH, Yao Q, Hui SE, Niu YQ (2018) N2O and NO formation from NH3 oxidation over MnO2/TiO2 catalysts. Fuel 234:650–655. https://doi.org/10.1016/j.fuel.2018.07.073
Wu ZB, Jiang B, Liu YQ, Wang HQ, Jin RB (2007) DRIFT study of manganese/titania-based catalysts for low-temperature selective catalytic reduction of NO with NH3. Environ Sci Technol 41:5812–5817. https://doi.org/10.1021/es0700350
Xu Q, Su RJ, Cao L, Li YQ, Yang CY, Luo Y, Street J, Jiao PC, Cai LL (2017) Facile preparation of high-performance Fe-doped Ce-Mn/TiO2 catalysts for the low-temperature selective catalytic reduction of NOx with NH3. RSC Adv. 7(77):48785–48792. https://doi.org/10.1039/C7RA07854D
Yan QH, Chen SN, Zhang C, O’Hare D, Wang Q (2018) Synthesis of Cu0.5Mg1.5Mn0.5Al0.5Ox mixed oxide from layered double hydroxide precursor as highly efficient catalyst for low-temperature selective catalytic reduction of NOx with NH3. J Colloid Interface Sci 526:63–74. https://doi.org/10.1016/j.jcis.2018.04.099
You XC, Sheng ZY, Yu DQ, Yang L, Xiao XX, Wang SS (2017) Influence of Mn/Ce ratio on the physicochemical properties and catalytic performance of graphene supported MnOx-CeO2 oxides for NH3-SCR at low temperature. Appl Surf Sci 423:845–854. https://doi.org/10.1016/j.apsusc.2017.06.226
Yu CL, Huang BC, Dong LF, Chen F, Liu XQ (2017) In situ FT-IR study of highly dispersed MnOx/SAPO-34 catalyst for low-temperature selective catalytic reduction of NOx by NH3. Catal Today 281:610–620. https://doi.org/10.1016/j.cattod.2016.06.025
Zhang L, Zhang DS, Zhang JP, Cai SX, Fang C, Huang L, Li HR, Gao RH, Shi LY (2013) Design of meso-TiO2@MnOx-CeOx/CNTs with a core-shell structure as DeNOx catalysts: promotion of activity, stability and SO2-tolerance. Nanoscale 5(20):9821–9829. https://doi.org/10.1039/c3nr03150k
Zhang SG, Zhang BL, Liu B, Sun SL (2017) A review of Mn-containing oxide catalysts for low temperature selective catalytic reduction of NOx with NH3: reaction mechanism and catalyst deactivation. RSC Adv 7(42):26226–26242. https://doi.org/10.1039/c7ra03387g
Zhang SB, Zhao YC, Yang JP, Zhang JY, Zheng CG (2018) Fe-modified MnOx/TiO2 as the SCR catalyst for simultaneous removal of NO and mercury from coal combustion flue gas. Chem Eng J 348:618–629. https://doi.org/10.1016/j.cej.2018.05.037
Zhou LL, Li CT, Zhao LK, Zeng GM, Gao L, Wang Y, Yu ME (2016) The poisoning effect of PbO on Mn-Ce/TiO2 catalyst for selective catalytic reduction of NO with NH3 at low temperature. Appl Surf Sci 389:532–539. https://doi.org/10.1016/j.apsusc.2016.07.136
Zhu LL, Huang BC, Wang WH, Wei ZL, Ye DQ (2011) Low-temperature SCR of NO with NH3 over CeO2 supported on modified activated carbon fibers. Catal Commun 12(6):394–398. https://doi.org/10.1016/j.catcom.2010.10.028
Zuo SF, Huang QQ, Li J, Zhou RX (2009) Promoting effect of Ce added to metal oxide supported on Al pillared clays for deep benzene oxidation. Appl Catal B-Environ 91(1-2):204–209. https://doi.org/10.1016/j.apcatb.2009.05.025
Funding
This study was funded by the National Key R&D Program of China (2017YFC0210303-01), the National Natural Science Foundation of China (21806009), the project funded by the China Postdoctoral Science Foundation (2018M631344), the Fundamental Research Funds for the Central Universities (FRF-TP-18-019A1), and the program “Promoting the Cooperative Innovation Among Beijing, Tianjin, and Hebei” (Z161100002716025).
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Gu, T., Gao, F., Tang, X. et al. Fe-modified Ce-MnOx/ACFN catalysts for selective catalytic reduction of NOx by NH3 at low-middle temperature. Environ Sci Pollut Res 26, 27940–27952 (2019). https://doi.org/10.1007/s11356-019-05976-4
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DOI: https://doi.org/10.1007/s11356-019-05976-4