摘要
The vanadium oxide/reduced graphene oxide(V_2 O_5/rGO) composite catalyst which determined the selective catalytic reduction activity(SCR) of NO with NH_3 was prepared by a simple solvothermal method. The physicochemical properties of the catalysts were characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM), Raman, X-ray energy spectrometer(XPS) and N_2 sorption isotherm measurement(BET). Results of NH_3-SCR showed that the NO conversion of V_2 O_5/rGO catalyst could reach 54.3% at 100 ℃. And the removal of NO increased to 74.6% when the temperature was up to 220 ℃. By characterizing the microstructure and morphology of the V_2 O_5/rGO catalysts prepared by in-situ growth and mechanical mixing methods, it was further shown that V_2 O_5 nanoparticles were highly dispersed and in situ growth on the rGO surface. Based on X-ray energy spectrometer, V_2 O_5/r GO catalyst had good low temperature denitrification performance due to the chemical adsorption oxygen and low-valent vanadium oxide contained in V_2 O_5/rGO catalyst, which was beneficial to the redox reaction between V_2 O_5 and graphene.
The vanadium oxide/reduced graphene oxide(V_2 O_5/rGO) composite catalyst which determined the selective catalytic reduction activity(SCR) of NO with NH_3 was prepared by a simple solvothermal method. The physicochemical properties of the catalysts were characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM), Raman, X-ray energy spectrometer(XPS) and N_2 sorption isotherm measurement(BET). Results of NH_3-SCR showed that the NO conversion of V_2 O_5/rGO catalyst could reach 54.3% at 100 ℃. And the removal of NO increased to 74.6% when the temperature was up to 220 ℃. By characterizing the microstructure and morphology of the V_2 O_5/rGO catalysts prepared by in-situ growth and mechanical mixing methods, it was further shown that V_2 O_5 nanoparticles were highly dispersed and in situ growth on the rGO surface. Based on X-ray energy spectrometer, V_2 O_5/r GO catalyst had good low temperature denitrification performance due to the chemical adsorption oxygen and low-valent vanadium oxide contained in V_2 O_5/rGO catalyst, which was beneficial to the redox reaction between V_2 O_5 and graphene.
引文
[1]Fang D,He F,Xie J,et al.Effects of Atmospheres and Precursors on MnOx/TiO2_ Catalysts for NH3-SCR at Low Temperature[J].Journal of Wuhan University of Technology-Materials Science Edition,2013,28(5):888-892
[2]Guan B,Zhan R,Lin H,et al.Review of State of the Art Technologies of Selective Catalytic Reduction of NOx from Diesel Engine Exhaust[J].Applied Thermal Engineering,2014,66(1):395-414
[3]Zhu L,Zhong Z,Xue J,et al.NH3-SCR Performance and the Resistance to SO_2 for Nb Doped Vanadium Based Catalyst at Low Temperatures[J].Journal of Environmental Sciences,2018,65:306-316
[4]Zhang S,Li H,Zhong Q.Promotional Effect of F-Doped V_2O_5-WO_3/TiO_2 Catalyst for NH3-SCR of NO at Low-Temperature[J].Applied Catalysis A:General,2012,435-436:156-162
[5]Arfaoui J,Ghorbel A,Petitto C,et al.Novel Vanadium Supported onto Mixed Molybdenum-Titanium Pillared Clay Catalysts for the Low Temperature SCR-NO by NH3[J].Chemical Engineering Journal,2017,356:598-608
[6]Song L,Zhang R,Zang S,et al.Activity of Selective Catalytic Reduction of NO over V_2O_5/TiO_2 Catalysts Preferentially Exposed Anatase{001}and{101}Facets[J].Catalysis Letters,2017,147(4):934-945
[7]Shi Q,Li Y,Zhou Y,et al.The Shape Effect of TiO2_ in VOx/TiO2_ Catalysts for Selective Reduction of NO by NH3[J].Journal of Materials Chemistry A,2015,3(27):14 409-14 415
[8]Chen C,Yue C,Liu S,et al.Review on the Latest Developments in Modified Vanadium-Titanium-Based SCR Catalysts[J].Chinese Journal of Catalysis,2018,39(8):1 347-1 365
[9]Shan W,Song H.Catalysts for the Selective Catalytic Reduction of NOx with NH3 at Low Temperature[J].Catalysis Science&Technology,2015,5(9):4 280-4 288
[10]Lu X,Song C,Jia S,et al.Low-Temperature Selective Catalytic Reduction of NOx with NH3 over Cerium and Manganese Oxides Supported on TiO2-Graphene[J].Chemical Engineering Journal,2015,260:776-784
[11]Lu X,Song C,Chang C C,et al.Manganese Oxides Supported on TiO2-Graphene Nanocomposite Catalysts for Selective Catalytic Reduction of NOx with NH3 at Low Temperature[J].Industrial&Engineering Chemistry Research,2014,53(29):11 601-11 610
[12]Xiao X,Sheng Z,Yang L,et al.Low-Temperature Selective Catalytic Reduction of NOx with NH3 over a Manganese and Cerium Oxide/Graphene Composite Prepared by a Hydrothermal Method[J].Catalysis Science&Technology,2016,6(5):1 507-1 514
[13]Gao F,Tang X,Yi H,et al.A Review on Selective Catalytic Reduction of NOx by NH3 over Mn-Based Catalysts at Low Temperatures:Catalysts,Mechanisms,Kinetics and DFT Calculations[J].Catalysts,2017,7(7):1-32
[14]Chuang X U,Bing X U,Jun H.Characterization and Saturable Absorption Property of Graphene Oxide on Optical Fiber by Optical Deposition[J].Journal of Wuhan University of Technology-Materials Science Edition,2017,4:140-145
[15]Dong Y,Niu X,Song W,et al.Facile Synthesis of Vanadium Oxide/Reduced Graphene Oxide Composite Catalysts for Enhanced Hydroxylation of Benzene to Phenol[J].Catalysts,2016,6(5):1-16
[16]Choo S T,Lee Y G,Nam I S,et al.Characteristics of V_2O_5 Supported on Sulfated TiO2_ for Selective Catalytic Reduction of NO by NH3[J].Applied Catalysis A:General,2000,200(1):177-188
[17]Mitran G,Ahmed R,Iro E,et al.Propane Oxidative Dehydrogenation over VOx/SBA-15 Catalysts[J].Catalysis Today,2018,306:260-267
[18]Bosco M V,Ba?ares M A,Martínez-Huerta M V,et al.In Situ FTIRand Raman Study on the Distribution and Reactivity of Surface Vanadia Species in V_2O_5/CeO2 Catalysts[J].Journal of Molecular Catalysis A:Chemical,2015,408:75-84
[19]Jiang L,Gao L.Modified Carbon Nanotubes:an Effective Way to Selective Attachment of Gold Nanoparticles[J].Carbon,2003,41(15):2 923-2 929
[20]Xiao L,Zhao M,Hu H.Study on Graphene Oxide Modified Inorganic Phase Change Materials and Their Packaging Behavior[J].Journal of Wuhan University of Technology-Material Science Edition,2018,33(4):788-792
[21]Cha W,Chin S,Park E,et al.Effect of V_2O_5 Loading of V_2O_5/TiO_2Catalysts Prepared via CVC and Impregnation Methods on NOx Removal[J].Applied Catalysis B:Environmental,2013,140-141:708-715
[22]Liu C,Shi J-W,Gao C,et al.Manganese Oxide-Based Catalysts for Low-Temperature Selective Catalytic Reduction of NOx with NH3:a Review[J].Applied Catalysis A:General,2016,522:54-69
[23]Kaichev V V,Chesalov Y A,Saraev A A,et al.Redox Mechanism for Selective Oxidation of Ethanol over Monolayer V_2O_5/TiO_2 Catalysts[J].Journal of Catalysis,2016,338:82-93
[24]Shan W,Liu F,He H,et al.A Superior Ce-W-Ti Mixed Oxide Catalyst for the Selective Catalytic Reduction of NOx with NH3[J].Applied Catalysis B:Environmental,2012,115-116:100-106
[25]Kwon D W,Park K H,Hong S C.Influence of VOx Surface Density and Vanadyl Species on the Selective Catalytic Reduction of NO by NH3 over VOx/TiO2_ for Superior Catalytic Activity[J].Applied Catalysis A:General,2015,499:1-12
[26]Yang X H,Fu H T,An X Z,et al.Synthesis of V_2O_5@TiO2_ Core-Shell Hybrid Composites for Sunlight Degradation of Methylene Blue[J].RSC Advances,2016,6(41):34 103-34 109
[27]Kumar P A,Jeong Y E,Ha H P.Low Temperature NH3-SCR Activity Enhancement of Antimony Promoted Vanadia-Ceria Catalyst[J].Catalysis Today,2017,293-294:61-72
[28]Huang B,Huang R,Jin D,et al.Low Temperature SCR of NO with NH3 over Carbon Nanotubes Supported Vanadium Oxides[J].Catalysis Today,2007,126(3-4):279-283
[29]Bai S,Jiang S,Li H,et al.Carbon Nanotubes Loaded with Vanadium Oxide for Reduction NO with NH3 at Low Temperature[J].Chinese Journal of Chemical Engineering,2015,23(3):516-519
[30]Zhang S,Zhong Q.Promotional Effect of WO3 on O2-over V_2O_5/TiO_2Catalyst for Selective Catalytic Reduction of NO with NH3[J].Journal of Molecular Catalysis A:Chemical,2013,373:108-113