CN108212146A - Nucleocapsid denitrating catalyst of metallic monoliths and preparation method thereof - Google Patents
Nucleocapsid denitrating catalyst of metallic monoliths and preparation method thereof Download PDFInfo
- Publication number
- CN108212146A CN108212146A CN201810017867.6A CN201810017867A CN108212146A CN 108212146 A CN108212146 A CN 108212146A CN 201810017867 A CN201810017867 A CN 201810017867A CN 108212146 A CN108212146 A CN 108212146A
- Authority
- CN
- China
- Prior art keywords
- salt
- nucleocapsid
- catalyst
- metallic
- denitrating catalyst
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
- 239000003054 catalyst Substances 0.000 title claims abstract description 85
- 238000002360 preparation method Methods 0.000 title claims abstract description 15
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 38
- 239000007822 coupling agent Substances 0.000 claims abstract description 36
- 239000012752 auxiliary agent Substances 0.000 claims abstract description 16
- 229910052751 metal Inorganic materials 0.000 claims abstract description 8
- 239000002184 metal Substances 0.000 claims abstract description 8
- 229910044991 metal oxide Inorganic materials 0.000 claims abstract description 5
- 150000004706 metal oxides Chemical class 0.000 claims abstract description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 claims abstract description 4
- 238000011065 in-situ storage Methods 0.000 claims abstract description 4
- 239000004411 aluminium Substances 0.000 claims description 45
- 229910052782 aluminium Inorganic materials 0.000 claims description 45
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 45
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 42
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 36
- VCJMYUPGQJHHFU-UHFFFAOYSA-N iron(3+);trinitrate Chemical compound [Fe+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O VCJMYUPGQJHHFU-UHFFFAOYSA-N 0.000 claims description 24
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 23
- 239000008367 deionised water Substances 0.000 claims description 21
- 229910021641 deionized water Inorganic materials 0.000 claims description 21
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 20
- 229910052759 nickel Inorganic materials 0.000 claims description 18
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical group O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 16
- 238000001027 hydrothermal synthesis Methods 0.000 claims description 16
- 239000000758 substrate Substances 0.000 claims description 13
- 150000003839 salts Chemical class 0.000 claims description 12
- 229910052726 zirconium Inorganic materials 0.000 claims description 11
- HSJPMRKMPBAUAU-UHFFFAOYSA-N cerium(3+);trinitrate Chemical compound [Ce+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O HSJPMRKMPBAUAU-UHFFFAOYSA-N 0.000 claims description 9
- 239000006260 foam Substances 0.000 claims description 9
- -1 mantoquita Chemical class 0.000 claims description 9
- 150000000703 Cerium Chemical class 0.000 claims description 8
- 239000003795 chemical substances by application Substances 0.000 claims description 8
- 239000002243 precursor Substances 0.000 claims description 8
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 7
- MCMNRKCIXSYSNV-UHFFFAOYSA-N ZrO2 Inorganic materials O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 7
- 229910052802 copper Inorganic materials 0.000 claims description 7
- 239000010949 copper Substances 0.000 claims description 7
- 150000002696 manganese Chemical class 0.000 claims description 7
- MIVBAHRSNUNMPP-UHFFFAOYSA-N manganese(2+);dinitrate Chemical compound [Mn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O MIVBAHRSNUNMPP-UHFFFAOYSA-N 0.000 claims description 7
- 238000000034 method Methods 0.000 claims description 7
- 229910052684 Cerium Inorganic materials 0.000 claims description 6
- 229910052742 iron Inorganic materials 0.000 claims description 6
- 239000011572 manganese Substances 0.000 claims description 6
- OERNJTNJEZOPIA-UHFFFAOYSA-N zirconium nitrate Chemical compound [Zr+4].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O OERNJTNJEZOPIA-UHFFFAOYSA-N 0.000 claims description 6
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 claims description 5
- UFMZWBIQTDUYBN-UHFFFAOYSA-N cobalt dinitrate Chemical compound [Co+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O UFMZWBIQTDUYBN-UHFFFAOYSA-N 0.000 claims description 5
- 229910001981 cobalt nitrate Inorganic materials 0.000 claims description 5
- 150000002148 esters Chemical class 0.000 claims description 5
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 4
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims description 4
- 229910021380 Manganese Chloride Inorganic materials 0.000 claims description 4
- GLFNIEUTAYBVOC-UHFFFAOYSA-L Manganese chloride Chemical compound Cl[Mn]Cl GLFNIEUTAYBVOC-UHFFFAOYSA-L 0.000 claims description 4
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 claims description 4
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 claims description 4
- 230000008859 change Effects 0.000 claims description 4
- 150000001868 cobalt Chemical class 0.000 claims description 4
- 229910017052 cobalt Inorganic materials 0.000 claims description 4
- 239000010941 cobalt Substances 0.000 claims description 4
- 125000002887 hydroxy group Chemical group [H]O* 0.000 claims description 4
- 150000002471 indium Chemical class 0.000 claims description 4
- RBTARNINKXHZNM-UHFFFAOYSA-K iron trichloride Chemical group Cl[Fe](Cl)Cl RBTARNINKXHZNM-UHFFFAOYSA-K 0.000 claims description 4
- 150000002603 lanthanum Chemical class 0.000 claims description 4
- FYDKNKUEBJQCCN-UHFFFAOYSA-N lanthanum(3+);trinitrate Chemical compound [La+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O FYDKNKUEBJQCCN-UHFFFAOYSA-N 0.000 claims description 4
- 229910052749 magnesium Inorganic materials 0.000 claims description 4
- 239000011777 magnesium Substances 0.000 claims description 4
- 239000011565 manganese chloride Substances 0.000 claims description 4
- 229940099607 manganese chloride Drugs 0.000 claims description 4
- 235000002867 manganese chloride Nutrition 0.000 claims description 4
- 150000002815 nickel Chemical class 0.000 claims description 4
- 150000003657 tungsten Chemical class 0.000 claims description 4
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 claims description 4
- 125000000218 acetic acid group Chemical group C(C)(=O)* 0.000 claims description 3
- VYLVYHXQOHJDJL-UHFFFAOYSA-K cerium trichloride Chemical compound Cl[Ce](Cl)Cl VYLVYHXQOHJDJL-UHFFFAOYSA-K 0.000 claims description 3
- VGBWDOLBWVJTRZ-UHFFFAOYSA-K cerium(3+);triacetate Chemical group [Ce+3].CC([O-])=O.CC([O-])=O.CC([O-])=O VGBWDOLBWVJTRZ-UHFFFAOYSA-K 0.000 claims description 3
- 229910052748 manganese Inorganic materials 0.000 claims description 3
- 229940071125 manganese acetate Drugs 0.000 claims description 3
- UOGMEBQRZBEZQT-UHFFFAOYSA-L manganese(2+);diacetate Chemical compound [Mn+2].CC([O-])=O.CC([O-])=O UOGMEBQRZBEZQT-UHFFFAOYSA-L 0.000 claims description 3
- HYZQBNDRDQEWAN-LNTINUHCSA-N (z)-4-hydroxypent-3-en-2-one;manganese(3+) Chemical compound [Mn+3].C\C(O)=C\C(C)=O.C\C(O)=C\C(C)=O.C\C(O)=C\C(C)=O HYZQBNDRDQEWAN-LNTINUHCSA-N 0.000 claims description 2
- 241001502050 Acis Species 0.000 claims description 2
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 claims description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 claims description 2
- 229910021586 Nickel(II) chloride Inorganic materials 0.000 claims description 2
- XURCIPRUUASYLR-UHFFFAOYSA-N Omeprazole sulfide Chemical compound N=1C2=CC(OC)=CC=C2NC=1SCC1=NC=C(C)C(OC)=C1C XURCIPRUUASYLR-UHFFFAOYSA-N 0.000 claims description 2
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 2
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims description 2
- 229910001297 Zn alloy Inorganic materials 0.000 claims description 2
- MQRWBMAEBQOWAF-UHFFFAOYSA-N acetic acid;nickel Chemical compound [Ni].CC(O)=O.CC(O)=O MQRWBMAEBQOWAF-UHFFFAOYSA-N 0.000 claims description 2
- 150000004645 aluminates Chemical class 0.000 claims description 2
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 2
- UNTBPXHCXVWYOI-UHFFFAOYSA-O azanium;oxido(dioxo)vanadium Chemical compound [NH4+].[O-][V](=O)=O UNTBPXHCXVWYOI-UHFFFAOYSA-O 0.000 claims description 2
- 239000006227 byproduct Substances 0.000 claims description 2
- 229940011182 cobalt acetate Drugs 0.000 claims description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 2
- GVPFVAHMJGGAJG-UHFFFAOYSA-L cobalt dichloride Chemical group [Cl-].[Cl-].[Co+2] GVPFVAHMJGGAJG-UHFFFAOYSA-L 0.000 claims description 2
- QAHREYKOYSIQPH-UHFFFAOYSA-L cobalt(II) acetate Chemical compound [Co+2].CC([O-])=O.CC([O-])=O QAHREYKOYSIQPH-UHFFFAOYSA-L 0.000 claims description 2
- 229910052681 coesite Inorganic materials 0.000 claims description 2
- 239000000470 constituent Substances 0.000 claims description 2
- ORTQZVOHEJQUHG-UHFFFAOYSA-L copper(II) chloride Chemical compound Cl[Cu]Cl ORTQZVOHEJQUHG-UHFFFAOYSA-L 0.000 claims description 2
- XTVVROIMIGLXTD-UHFFFAOYSA-N copper(II) nitrate Chemical compound [Cu+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O XTVVROIMIGLXTD-UHFFFAOYSA-N 0.000 claims description 2
- 229910052593 corundum Inorganic materials 0.000 claims description 2
- 229910052906 cristobalite Inorganic materials 0.000 claims description 2
- VBXWCGWXDOBUQZ-UHFFFAOYSA-K diacetyloxyindiganyl acetate Chemical compound [In+3].CC([O-])=O.CC([O-])=O.CC([O-])=O VBXWCGWXDOBUQZ-UHFFFAOYSA-K 0.000 claims description 2
- 235000019441 ethanol Nutrition 0.000 claims description 2
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims description 2
- 229910052737 gold Inorganic materials 0.000 claims description 2
- 239000010931 gold Substances 0.000 claims description 2
- 229910052738 indium Inorganic materials 0.000 claims description 2
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 claims description 2
- FBAFATDZDUQKNH-UHFFFAOYSA-M iron chloride Chemical group [Cl-].[Fe] FBAFATDZDUQKNH-UHFFFAOYSA-M 0.000 claims description 2
- PVFSDGKDKFSOTB-UHFFFAOYSA-K iron(3+);triacetate Chemical compound [Fe+3].CC([O-])=O.CC([O-])=O.CC([O-])=O PVFSDGKDKFSOTB-UHFFFAOYSA-K 0.000 claims description 2
- 229910052746 lanthanum Inorganic materials 0.000 claims description 2
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 claims description 2
- JLRJWBUSTKIQQH-UHFFFAOYSA-K lanthanum(3+);triacetate Chemical group [La+3].CC([O-])=O.CC([O-])=O.CC([O-])=O JLRJWBUSTKIQQH-UHFFFAOYSA-K 0.000 claims description 2
- ICAKDTKJOYSXGC-UHFFFAOYSA-K lanthanum(iii) chloride Chemical compound Cl[La](Cl)Cl ICAKDTKJOYSXGC-UHFFFAOYSA-K 0.000 claims description 2
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 claims description 2
- 229910000000 metal hydroxide Inorganic materials 0.000 claims description 2
- 150000004692 metal hydroxides Chemical class 0.000 claims description 2
- 229940078494 nickel acetate Drugs 0.000 claims description 2
- QMMRZOWCJAIUJA-UHFFFAOYSA-L nickel dichloride Chemical group Cl[Ni]Cl QMMRZOWCJAIUJA-UHFFFAOYSA-L 0.000 claims description 2
- KBJMLQFLOWQJNF-UHFFFAOYSA-N nickel(ii) nitrate Chemical compound [Ni+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O KBJMLQFLOWQJNF-UHFFFAOYSA-N 0.000 claims description 2
- 239000003960 organic solvent Substances 0.000 claims description 2
- IYDGMDWEHDFVQI-UHFFFAOYSA-N phosphoric acid;trioxotungsten Chemical compound O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.O=[W](=O)=O.OP(O)(O)=O IYDGMDWEHDFVQI-UHFFFAOYSA-N 0.000 claims description 2
- 229910052710 silicon Inorganic materials 0.000 claims description 2
- 239000010703 silicon Substances 0.000 claims description 2
- 239000000377 silicon dioxide Substances 0.000 claims description 2
- 229910052682 stishovite Inorganic materials 0.000 claims description 2
- 229910052905 tridymite Inorganic materials 0.000 claims description 2
- 229910052721 tungsten Inorganic materials 0.000 claims description 2
- 239000010937 tungsten Substances 0.000 claims description 2
- 229910052720 vanadium Inorganic materials 0.000 claims description 2
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 claims description 2
- 229910001845 yogo sapphire Inorganic materials 0.000 claims description 2
- 229910052725 zinc Inorganic materials 0.000 claims description 2
- 239000011701 zinc Substances 0.000 claims description 2
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 claims 1
- 239000000460 chlorine Substances 0.000 claims 1
- 229910052801 chlorine Inorganic materials 0.000 claims 1
- 230000003647 oxidation Effects 0.000 claims 1
- 238000007254 oxidation reaction Methods 0.000 claims 1
- 235000021419 vinegar Nutrition 0.000 claims 1
- 239000000052 vinegar Substances 0.000 claims 1
- ZXAUZSQITFJWPS-UHFFFAOYSA-J zirconium(4+);disulfate Chemical compound [Zr+4].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O ZXAUZSQITFJWPS-UHFFFAOYSA-J 0.000 claims 1
- 230000000694 effects Effects 0.000 abstract description 36
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 abstract description 20
- 239000000463 material Substances 0.000 abstract description 13
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 abstract description 8
- 229910052717 sulfur Inorganic materials 0.000 abstract description 6
- 239000011593 sulfur Substances 0.000 abstract description 6
- 230000008901 benefit Effects 0.000 abstract description 3
- 229910000831 Steel Inorganic materials 0.000 abstract description 2
- 239000007789 gas Substances 0.000 abstract description 2
- 238000000465 moulding Methods 0.000 abstract description 2
- 238000012545 processing Methods 0.000 abstract description 2
- 230000001846 repelling effect Effects 0.000 abstract description 2
- 239000010959 steel Substances 0.000 abstract description 2
- 239000002699 waste material Substances 0.000 abstract 1
- 229910001593 boehmite Inorganic materials 0.000 description 30
- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 description 30
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 24
- 238000006243 chemical reaction Methods 0.000 description 23
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 14
- 230000003197 catalytic effect Effects 0.000 description 14
- 239000003546 flue gas Substances 0.000 description 14
- 239000002131 composite material Substances 0.000 description 12
- 238000005470 impregnation Methods 0.000 description 12
- 239000011259 mixed solution Substances 0.000 description 12
- 239000000203 mixture Substances 0.000 description 12
- 229910052757 nitrogen Inorganic materials 0.000 description 12
- IJGRMHOSHXDMSA-UHFFFAOYSA-N nitrogen Substances N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 12
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 12
- 239000010453 quartz Substances 0.000 description 12
- 238000012360 testing method Methods 0.000 description 12
- 238000002604 ultrasonography Methods 0.000 description 12
- 239000003643 water by type Substances 0.000 description 12
- 239000000243 solution Substances 0.000 description 10
- 238000005406 washing Methods 0.000 description 9
- 239000004408 titanium dioxide Substances 0.000 description 8
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 5
- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonia chloride Chemical compound [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 description 4
- ZGMCLEXFYGHRTK-UHFFFAOYSA-N [Fe].[Ce] Chemical compound [Fe].[Ce] ZGMCLEXFYGHRTK-UHFFFAOYSA-N 0.000 description 4
- JKQOBWVOAYFWKG-UHFFFAOYSA-N molybdenum trioxide Chemical compound O=[Mo](=O)=O JKQOBWVOAYFWKG-UHFFFAOYSA-N 0.000 description 4
- BFDHFSHZJLFAMC-UHFFFAOYSA-L nickel(ii) hydroxide Chemical compound [OH-].[OH-].[Ni+2] BFDHFSHZJLFAMC-UHFFFAOYSA-L 0.000 description 4
- 239000002253 acid Substances 0.000 description 3
- 238000006555 catalytic reaction Methods 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Natural products CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical group [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 2
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 2
- 239000005864 Sulphur Substances 0.000 description 2
- 235000019270 ammonium chloride Nutrition 0.000 description 2
- 239000012298 atmosphere Substances 0.000 description 2
- 238000006477 desulfuration reaction Methods 0.000 description 2
- 230000023556 desulfurization Effects 0.000 description 2
- NNLJGFCRHBKPPJ-UHFFFAOYSA-N iron lanthanum Chemical compound [Fe].[La] NNLJGFCRHBKPPJ-UHFFFAOYSA-N 0.000 description 2
- 239000010410 layer Substances 0.000 description 2
- 229910017604 nitric acid Inorganic materials 0.000 description 2
- 238000005303 weighing Methods 0.000 description 2
- 241000196324 Embryophyta Species 0.000 description 1
- 241000264877 Hippospongia communis Species 0.000 description 1
- QVYYOKWPCQYKEY-UHFFFAOYSA-N [Fe].[Co] Chemical compound [Fe].[Co] QVYYOKWPCQYKEY-UHFFFAOYSA-N 0.000 description 1
- WYCDUUBJSAUXFS-UHFFFAOYSA-N [Mn].[Ce] Chemical compound [Mn].[Ce] WYCDUUBJSAUXFS-UHFFFAOYSA-N 0.000 description 1
- VQWQYXBWRCCZGX-UHFFFAOYSA-N acetic acid;manganese Chemical compound [Mn].CC(O)=O.CC(O)=O VQWQYXBWRCCZGX-UHFFFAOYSA-N 0.000 description 1
- 238000003916 acid precipitation Methods 0.000 description 1
- 230000003321 amplification Effects 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 238000010531 catalytic reduction reaction Methods 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 239000003426 co-catalyst Substances 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 239000011247 coating layer Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- OPQARKPSCNTWTJ-UHFFFAOYSA-L copper(ii) acetate Chemical compound [Cu+2].CC([O-])=O.CC([O-])=O OPQARKPSCNTWTJ-UHFFFAOYSA-L 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
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- 230000007613 environmental effect Effects 0.000 description 1
- 231100000584 environmental toxicity Toxicity 0.000 description 1
- 238000001125 extrusion Methods 0.000 description 1
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- 239000012943 hotmelt Substances 0.000 description 1
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- 239000006262 metallic foam Substances 0.000 description 1
- 238000003199 nucleic acid amplification method Methods 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- CMOAHYOGLLEOGO-UHFFFAOYSA-N oxozirconium;dihydrochloride Chemical compound Cl.Cl.[Zr]=O CMOAHYOGLLEOGO-UHFFFAOYSA-N 0.000 description 1
- 231100000572 poisoning Toxicity 0.000 description 1
- 230000000607 poisoning effect Effects 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- WKXHZKXPFJNBIY-UHFFFAOYSA-N titanium tungsten vanadium Chemical compound [Ti][W][V] WKXHZKXPFJNBIY-UHFFFAOYSA-N 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
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Abstract
Nucleocapsid denitrating catalyst the invention discloses a kind of metallic monoliths and preparation method thereof.The denitrating catalyst is the growth in situ hydroxide on metallic monolith carrier, is then self-assembled into the catalyst with core-casing structure of metallic monoliths by one step of two-way bridge linking effect of coupling agent, wherein main active component and auxiliary agent are core, metal is oxidized to shell.Main activity component load quantity is 0.01 ~ 30 wt%, and auxiliary agent load capacity is 0 ~ 30 wt%, and metal oxide supported amount is 0 ~ 50 wt%, and surplus is metal integral material.Catalyst of the present invention has many advantages, such as that low temperature active is good, sulfur resistive water repelling property is excellent, preparation method is simple, good without molding, thermal conductivity, the processing of the nitrogen oxides suitable for the tail gas of the discharges such as coal-burning power plant, waste incinerator and steel mill.
Description
Technical field
The present invention relates to a kind of denitrating catalysts and preparation method thereof, and particularly one kind is using metallic monolith carrier as raw material
The nucleocapsid denitrating catalyst of metallic monoliths and preparation method thereof, which is suitable for that operating mode is complicated to be contained
SO2With the removal of nitrogen oxide of the fixation source emission of steam, belong to nitrogen oxides control and purification techniques field in environmental protection.
Background technology
With industry and economic rapid development, the flue gas of coal-burning power plant, steel plant and boiler factory's discharge causes air
Very big pollution.Nitrogen oxides（NOx）It is the important root of acid rain, photochemical fog, haze as main atmosphere pollution,
Grave danger is formed to the ecosystem and health.Ammine selectivity catalytic reduction（NH3-SCR）Be domestic and international application the most
Extensive gas denitrifying technology, catalyst are then the cores of the reaction.V at present2O5-WO3(MoO3)/TiO2Catalyst has realized quotient
Industry, however the catalyst activity temperature window is higher（300~400oC）, therefore catalytic unit need to be placed in dedusting, desulfurization it
Before, to ensure hot conditions, but dusty and high SO2Atmosphere easily leads to catalyst poisoning inactivation.If however denitration is placed in and is removed
After dirt desulfurization, flue-gas temperature is usually relatively low, catalyst activity degradation.Therefore it is badly in need of high efficient cryogenic sulfur resistive SCR to be developed
Catalyst.
Traditional V2O5-WO3(MoO3)/TiO2Catalyst is generally required in practical application to carry out extrusion forming or is coated in
On some molding carriers, such as ceramic honey comb or activated carbon, but these carrier thermal responses are slow, mass-transfer performance is low, easily by
The influences such as dust, service life are short.In recent years, metallic carrier has many advantages, such as that exhaust resistance is small, thermal conductivity is high, hot melt is small and obtains
To more and more concerns.Chinese patent CN100455352C and Chinese patent CN102166515A disclose aluminum oxide coating layer
The TiO of Cellulated wiremesh load2Or WO3-TiO2Catalyst, but paint-on technique is related to the secondary of catalyst activity component
Load has the shortcomings that complex steps, processing cost are high, coating is uneven, catalyst is easy to fall off, it is difficult to adapt to complicated operating mode
Using, and also without solving the defects of low temperature sulfur resistance is poor at all, therefore urgently exploitation new type low temperature sulfur resistive metal is whole
The technology of preparing of formula denitrating catalyst.
Invention content
It is an object of the present invention to overcome problems of the prior art, it is proposed that a kind of metallic monoliths
Nucleocapsid denitrating catalyst.
The second object of the present invention is to provide the preparation method of the denitrating catalyst.
In order to achieve the above objectives, the present invention adopts the following technical scheme that：
The nucleocapsid denitrating catalyst of a kind of metallic monoliths, it is characterised in that the denitrating catalyst is with monoblock type gold
It is core to belong to for carrier, the main active component of area load and auxiliary agent, and catalyst of the metal oxide for the nucleocapsid of shell is lived
Property component and auxiliary agent grain size be 1-30 nm；The auxiliary agent and the mass ratio of main active component are 0-0.01；The core with
The mass ratio of shell is 0.1-10.
Above-mentioned integral type metal carrier is aluminium, iron, magnesium, nickel, copper, zinc or containing aluminium, iron, magnesium, nickel, copper, zinc alloy
Woven wire or metal foam.
Above-mentioned main active component is one kind of Fe, Mn, Ce.
Above-mentioned auxiliary agent is at least one of manganese, lanthanum, indium, cobalt, copper, nickel, cerium, tungsten, zirconium, vanadium.
Above-mentioned metal oxide is SiO2、Al2O3、TiO2、ZrO2At least one.
A kind of method of nucleocapsid denitrating catalyst for preparing above-mentioned metallic monoliths, it is characterised in that the party
Method the specific steps are：
A. metallic monolith carrier is subjected to hydro-thermal reaction, its surface in situ is made to grow one layer of metal hydroxides；
B. main active component precursor salt, auxiliary agent precursor salt and coupling agent are dissolved in by the mass ratio of 0.1-10 in organic solution, filled
Divide and be uniformly mixed, the coupling agent Ao that homogeneous transparent is made closes solution；
C. by step a obtained by product, be impregnated in coupling agent Ao obtained by step b and close in solution, stand 0.5~4 h, instill
Deionized water, standing 0.5 ~ 5 h makes coupling agent be fully hydrolyzed with the hydroxyl in the hydroxide on monolithic substrate, dries
Afterwards, the catalyst with core-casing structure of metallic monoliths is made in 300-600 DEG C of roasting temperature 3-5 h.
Above-mentioned main active component precursor salt is molysite, manganese salt or cerium salt.
Above-mentioned molysite is iron chloride, ferric acetate, ferric nitrate or ferric acetyl acetonade；The manganese salt is manganese chloride, acetic acid
Manganese, manganese nitrate or manganese acetylacetonate；The cerium salt is cerous acetate, cerous nitrate or cerium chloride；Main active constituent is relative to metal
The load capacity of monolithic substrate is 0.01-30 wt%.
Above-mentioned auxiliary agent precursor salt is manganese salt, in lanthanum salt, indium salts, cobalt salt, mantoquita, nickel salt, cerium salt, tungsten salt, zirconates, vanadic salts
At least one.
Above-mentioned manganese salt is manganese chloride, one kind in manganese acetate, manganese nitrate；Lanthanum salt is lanthanum acetate, lanthanum nitrate, lanthanum chloride
It is a kind of；Indium salts are indium acetate, one kind of indium nitrate, inidum chloride；Cobalt salt is cobalt chloride, one kind in cobalt acetate, cobalt nitrate；Mantoquita
For one kind in copper chloride, copper acetate, copper nitrate；Nickel salt is nickel chloride, one kind in nickel acetate, nickel nitrate；Cerium salt is acetic acid
One kind in cerium, cerous nitrate, cerium chloride；Tungsten salt is ammonium tungstate, one kind in ammonium metatungstate, phosphotungstic acid；Zirconates is zirconium nitrate, sulphur
One kind in sour zirconium, zirconium oxychloride；Vanadic salts is ammonium metavanadate；Auxiliary agent is 0-30 relative to the load capacity of metallic monolith carrier
wt%。
Above-mentioned coupling agent for esters of silicon acis coupling agent, aluminate coupling agent, titanate coupling agent, zirconium ester coupling agent one
Kind.Shell oxide is 0-50 wt% relative to the load capacity of metallic monolith carrier.
The temperature of above-mentioned hydro-thermal reaction is 60~180oC, hydro-thermal time are 1~36 h.
Above-mentioned organic solvent is methanol, one kind in acetone, ethyl alcohol.
The dosage of above-mentioned deionized water is 10~50 wt% of metallic monolith carrier quality.
Compared with prior art, the present invention its advantage is as follows：
（1）Compared with traditional paint-on technique prepares integral catalyzer, the preparation of this integral catalyzer is simply easy to industrial amplification,
Growth in situ makes its Catalytic Layer not easily to fall off.Metal generally carrier, pressure drop is low, thermal conductivity is more preferable.
（2）This integral catalyzer has environmental toxicity small compared with traditional vanadium tungsten titanium catalyst, and low temperature active is high, resists
Sulphur water repelling property is excellent, is more suitable for the denitration application of operating mode complexity.
Description of the drawings
Fig. 1 is the sulfur resistive activity of the ferrum-cobalt catalyst of the titanium dioxide package of the aluminium wire netting structuring prepared by example IV
With sulfur resistive, water resistant stability curve.
Specific embodiment
In order to illustrate more clearly of the present invention, following embodiment is enumerated, but the enforceable situation of the present invention is not limited in
The range of embodiment.
Embodiment one：1 g aluminium wire nettings are placed in the hydrothermal reaction kettle containing deionized water, 100o12 h of C hydro-thermals.Go from
Sub- water washing 3 times, 100oC dries 12 h, and the boehmite composite material of aluminium wire netting structuring is made.It weighs containing 0.1 g
The cerous nitrate of the ferric nitrate of Fe and 0.03 g Ce are dissolved in 0.8 g methanol, add in the bis- triethanolamine diisopropyl titaniums of 0.416 g
Acid esters, ultrasound 10 minutes.Then it is small to be stood 2 in above-mentioned mixed solution for the boehmite incipient wetness impregnation of aluminium wire netting structuring
Shi Hou instills 0.08 g deionized waters, and standing 4 h makes coupling agent that abundant water occur with the boehmite on monolithic substrate
Solution.Resulting materials 100oC dries 12 h, 500oCRoast the iron cerium catalysis that the titanium dioxide package of aluminium wire netting structuring is made in 3 h
Agent.
The catalytic activity of above-mentioned catalyst is tested, simulated flue gas is by N2、O2、NO、NH3、SO2Composition, wherein NO, NH3、SO2
Volumetric concentration is 500 ppm, O2A concentration of 3%, Balance Air is nitrogen.0.5 g is taken to be put into fixation the catalyst for preparing completion
Active testing is carried out in bed quartz tube reactor, in reaction temperature 90 ~ 510oC, air speed are 20000 h-1Under conditions of,
250-420 oMore than 90% NO removal efficiencies, and N can be achieved between C2Selectivity is 100%.The catalyst is 270oC、SO2
During a concentration of 500 ppm, NO conversion ratios are 98%, and 24 h activity are basically unchanged, and are passed through 10% steam, and activity drops to 96% or so
And maintain 12 h constant, steam is turned off rear activity and improved to 98% NO removal efficiencies.
Embodiment two：1 g aluminium wire nettings are placed in the hydrothermal reaction kettle containing deionized water, 100o12 h of C hydro-thermals.Go from
Sub- water washing 3 times, 100oC dries 12 h, and the boehmite composite material of aluminium wire netting structuring is made.It weighs containing 0.1 g
The zirconium nitrate of the ferric nitrate of Fe and 0.03 g Zr are dissolved in 0.8 g methanol, add in the bis- triethanolamine diisopropyl titaniums of 0.416 g
Acid esters, ultrasound 10 minutes.Then it is small to be stood 2 in above-mentioned mixed solution for the boehmite incipient wetness impregnation of aluminium wire netting structuring
Shi Hou instills 0.08 g deionized waters, and standing 4 h makes coupling agent that abundant water occur with the boehmite on monolithic substrate
Solution.Resulting materials 100oC dries 12 h, 500oCRoast the ferrozirconium catalysis that the titanium dioxide package of aluminium wire netting structuring is made in 3 h
Agent.
The catalytic activity of above-mentioned catalyst is tested, simulated flue gas is by N2、O2、NO、NH3、SO2Composition, wherein NO, NH3、SO2
Volumetric concentration is 500 ppm, O2A concentration of 3%, Balance Air is nitrogen.0.5 g is taken to be put into fixation the catalyst for preparing completion
Active testing is carried out in bed quartz tube reactor, in reaction temperature 90 ~ 510oC, air speed are 20000 h-1Under conditions of,
300-420 oAchievable more than 90% NO removal efficiencies between C, 300oBelow C N2Selectivity is 100%.The catalyst is 270oC、SO2During a concentration of 500 ppm, NO conversion ratios are 99%, and 24 h activity are basically unchanged, and are passed through 10% steam, and activity drops to 97%
It controls and maintains 12 h constant, steam is turned off rear activity and improved to 99% NO removal efficiencies.
Embodiment three：1 g aluminium wire nettings are placed in the hydrothermal reaction kettle containing deionized water, 100o12 h of C hydro-thermals.Go from
Sub- water washing 3 times, 100oC dries 12 h, and the boehmite composite material of aluminium wire netting structuring is made.It weighs containing 0.1 g
The lanthanum nitrate of the ferric nitrate of Fe and 0.03 g La are dissolved in 0.8 g methanol, add in the bis- triethanolamine diisopropyl titaniums of 0.416 g
Acid esters, ultrasound 10 minutes.Then it is small to be stood 2 in above-mentioned mixed solution for the boehmite incipient wetness impregnation of aluminium wire netting structuring
Shi Hou instills 0.08 g deionized waters, and standing 4 h makes coupling agent that abundant water occur with the boehmite on monolithic substrate
Solution.Resulting materials 100oC dries 12 h, 500oCRoast the iron lanthanum catalysis that the titanium dioxide package of aluminium wire netting structuring is made in 3 h
Agent.
The catalytic activity of above-mentioned catalyst is tested, simulated flue gas is by N2、O2、NO、NH3、SO2Composition, wherein NO, NH3、SO2
Volumetric concentration is 500 ppm, O2A concentration of 3%, Balance Air is nitrogen.0.5 g is taken to be put into fixation the catalyst for preparing completion
Active testing is carried out in bed quartz tube reactor, in reaction temperature 90 ~ 510oC, air speed are 20000 h-1Under conditions of,
270-420 oAchievable more than 90% NO removal efficiencies between C, 350oBelow C N2Selectivity is 100%.The catalyst is 270oC、SO2During a concentration of 500 ppm, NO conversion ratios are 95%, and 24 h activity are basically unchanged, and are passed through 10% steam, and activity drops to 92%
It controls and maintains 12 h constant, steam is turned off rear activity and improved to 95% NO removal efficiencies.
Example IV：
1 g aluminium wire nettings are placed in the hydrothermal reaction kettle containing deionized water, 100o12 h of C hydro-thermals.Deionized water is washed 3 times,
100 oC dries 12 h, and the boehmite composite material of aluminium wire netting structuring is made.Weigh containing 0.1 g Fe ferric nitrate and
The cobalt nitrate of 0.03 g Co is dissolved in 0.8 g methanol, adds in the bis- triethanolamine diisopropyl titanate esters of 0.416 g, ultrasound 10
Minute.Then the boehmite incipient wetness impregnation of aluminium wire netting structuring after standing 2 hours, is instilled in above-mentioned mixed solution
0.08 g deionized waters, make coupling agent be fully hydrolyzed with the boehmite on monolithic substrate.Resulting materials 100oC
Dry 12 h, 500 oCRoast the ferrum-cobalt catalyst that the titanium dioxide package of aluminium wire netting structuring is made in 3 h.
The catalytic activity of above-mentioned catalyst is tested, simulated flue gas is by N2、O2、NO、NH3、SO2Composition, wherein NO, NH3、SO2
Volumetric concentration is 500 ppm, O2A concentration of 3%, Balance Air is nitrogen.0.5 g is taken to be put into fixation the catalyst for preparing completion
Active testing is carried out in bed quartz tube reactor, as a result as shown in figure.In reaction temperature 90 ~ 510oC, air speed are 20000 h-1Under conditions of, in 240-420oMore than 90% removal of nitrogen oxide rate, and N can be kept between C2Selectivity is 100%.It should
Catalyst is 240oC、SO2During a concentration of 500 ppm, NO conversion ratios are basically unchanged close to 100%, and 24 h activity, are passed through 10%
Steam, activity drops to 97% or so and maintains 12 h constant, and rear activity of steam turning off is improved to the NO removings close to 100%
Rate.
Embodiment five：
1 g aluminium wire nettings are placed in the hydrothermal reaction kettle containing deionized water, 100o12 h of C hydro-thermals.Deionized water is washed 3 times,
100 oC dries 12 h, and the boehmite composite material of aluminium wire netting structuring is made.Weigh containing 0.1 g Mn manganese nitrate and
The cobalt nitrate of 0.03 g Co is dissolved in 0.8 g methanol, adds in the bis- triethanolamine diisopropyl titanate esters of 0.416 g, ultrasound 10
Minute.Then the boehmite incipient wetness impregnation of aluminium wire netting structuring after standing 2 hours, is instilled in above-mentioned mixed solution
0.08 g deionized waters, make coupling agent be fully hydrolyzed with the boehmite on monolithic substrate.Resulting materials 100oC
Dry 12 h, 500 oCRoast the manganese Co catalysts that the titanium dioxide package of aluminium wire netting structuring is made in 3 h.
The catalytic activity of above-mentioned catalyst is tested, simulated flue gas is by N2、O2、NO、NH3、SO2Composition, wherein NO, NH3、SO2
Volumetric concentration is 500 ppm, O2A concentration of 3%, Balance Air is nitrogen.0.5 g is taken to be put into fixation the catalyst for preparing completion
Active testing is carried out in bed quartz tube reactor, in reaction temperature 90 ~ 510oC, air speed are 20000 h-1Under conditions of,
210-420 oMore than 90% removal of nitrogen oxide rate can be kept between C, there is preferable low temperature active and wider temperature
Window.
Embodiment six：
1 g aluminium wire nettings are placed in the hydrothermal reaction kettle containing deionized water, 100o12 h of C hydro-thermals.Deionized water is washed 3 times,
100 oC dries 12 h, and the boehmite composite material of aluminium wire netting structuring is made.Weigh containing 0.1 g Mn manganese nitrate and
The cerous nitrate of 0.03 g Ce is dissolved in 0.8 g methanol, adds in the bis- triethanolamine diisopropyl titanate esters of 0.416 g, ultrasound 10
Minute.Then the boehmite incipient wetness impregnation of aluminium wire netting structuring after standing 2 hours, is instilled in above-mentioned mixed solution
0.08 g deionized waters, make coupling agent be fully hydrolyzed with the boehmite on monolithic substrate.Resulting materials 100oC
Dry 12 h, 500 oCRoast the manganese cerium catalyst that the titanium dioxide package of aluminium wire netting structuring is made in 3 h.
The catalytic activity of above-mentioned catalyst is tested, simulated flue gas is by N2、O2、NO、NH3、SO2Composition, wherein NO, NH3、SO2
Volumetric concentration is 500 ppm, O2A concentration of 3%, Balance Air is nitrogen.0.5 g is taken to be put into fixation the catalyst for preparing completion
Active testing is carried out in bed quartz tube reactor, in reaction temperature 90 ~ 510oC, air speed are 20000 h-1Under conditions of,
230-420 oMore than 90% removal of nitrogen oxide rate can be kept between C, there is preferable low temperature active and wider temperature
Window.
Embodiment seven：1 g aluminium wire nettings are placed in the hydrothermal reaction kettle containing deionized water, 100o12 h of C hydro-thermals.Go from
Sub- water washing 3 times, 100oC dries 12 h, and the boehmite composite material of aluminium wire netting structuring is made.It weighs containing 0.1 g
The cerous nitrate of the ferric nitrate of Fe and 0.03 g Ce are dissolved in 0.8 g methanol, add in 0.26 g zirconium ester coupling agents（ZCA-
N44）, ultrasound 10 minutes.Then it is small to be stood 2 in above-mentioned mixed solution for the boehmite incipient wetness impregnation of aluminium wire netting structuring
Shi Hou instills 0.08 g deionized waters, and standing 4 h makes coupling agent that abundant water occur with the boehmite on monolithic substrate
Solution.Resulting materials 100oC dries 12 h, 500 oCThe iron cerium for roasting the zirconium dioxide package that aluminium wire netting structuring is made in 3 h is urged
Agent.
The catalytic activity of above-mentioned catalyst is tested, simulated flue gas is by N2、O2、NO、NH3、SO2Composition, wherein NO, NH3、SO2
Volumetric concentration is 500 ppm, O2A concentration of 3%, Balance Air is nitrogen.0.5 g is taken to be put into fixation the catalyst for preparing completion
Active testing is carried out in bed quartz tube reactor, in reaction temperature 90 ~ 510oC, air speed are 20000 h-1Under conditions of,
300-360 oMore than 90% NO removal efficiencies, and N can be achieved between C2Selectivity is 100%.The catalyst is 270oC、SO2
During a concentration of 500 ppm, NO conversion ratios are 97%, and 24 h activity are basically unchanged, and are passed through 10% steam, and activity drops to 96% or so
And maintain 12 h constant, steam is turned off rear activity and improved to 97% NO removal efficiencies.
Embodiment eight：1 g aluminium wire nettings are placed in the hydrothermal reaction kettle containing deionized water, 100o12 h of C hydro-thermals.Go from
Sub- water washing 3 times, 100oC dries 12 h, and the boehmite composite material of aluminium wire netting structuring is made.It weighs containing 0.1 g
The manganese nitrate of the ferric nitrate of Fe and 0.03 g Mn are dissolved in 0.8 g methanol, add in 0.26 g zirconium ester coupling agents（ZCA-
N44）, ultrasound 10 minutes.Then it is small to be stood 2 in above-mentioned mixed solution for the boehmite incipient wetness impregnation of aluminium wire netting structuring
Shi Hou instills 0.08 g deionized waters, and standing 4 h makes coupling agent that abundant water occur with the boehmite on monolithic substrate
Solution.Resulting materials 100oC dries 12 h, 500 oCThe ferrimanganic for roasting the zirconium dioxide package that aluminium wire netting structuring is made in 3 h is urged
Agent.
The catalytic activity of above-mentioned catalyst is tested, simulated flue gas is by N2、O2、NO、NH3、SO2Composition, wherein NO, NH3、SO2
Volumetric concentration is 500 ppm, O2A concentration of 3%, Balance Air is nitrogen.0.5 g is taken to be put into fixation the catalyst for preparing completion
Active testing is carried out in bed quartz tube reactor, in reaction temperature 90 ~ 510oC, air speed are 20000 h-1Under conditions of,
270-360 oMore than 90% NO removal efficiencies, and N can be achieved between C2Selectivity is 100%.The catalyst is 270oC、SO2
During a concentration of 500 ppm, NO conversion ratios are 99%, and 24 h activity are basically unchanged, and are passed through 10% steam, and activity drops to 98% or so
And maintain 12 h constant, steam is turned off rear activity and improved to 99% NO removal efficiencies.
Embodiment nine：1 g aluminium wire nettings are placed in the hydrothermal reaction kettle containing deionized water, 100o12 h of C hydro-thermals.Go from
Sub- water washing 3 times, 100oC dries 12 h, and the boehmite composite material of aluminium wire netting structuring is made.It weighs containing 0.1 g
The lanthanum nitrate of the ferric nitrate of Fe and 0.03 g La are dissolved in 0.8 g methanol, add in 0.26 g zirconium ester coupling agents（ZCA-
N44）, ultrasound 10 minutes.Then it is small to be stood 2 in above-mentioned mixed solution for the boehmite incipient wetness impregnation of aluminium wire netting structuring
Shi Hou instills 0.08 g deionized waters, and standing 4 h makes coupling agent that abundant water occur with the boehmite on monolithic substrate
Solution.Resulting materials 100oC dries 12 h, 500 oCThe iron lanthanum for roasting the zirconium dioxide package that aluminium wire netting structuring is made in 3 h is urged
Agent.
The catalytic activity of above-mentioned catalyst is tested, simulated flue gas is by N2、O2、NO、NH3、SO2Composition, wherein NO, NH3、SO2
Volumetric concentration is 500 ppm, O2A concentration of 3%, Balance Air is nitrogen.0.5 g is taken to be put into fixation the catalyst for preparing completion
Active testing is carried out in bed quartz tube reactor, in reaction temperature 90 ~ 510oC, air speed are 20000 h-1Under conditions of,
270-360 oMore than 90% NO removal efficiencies, and N can be achieved between C2Selectivity is 100%.The catalyst is 270oC、SO2
During a concentration of 500 ppm, NO conversion ratios are 98%, and 24 h activity are basically unchanged, and are passed through 10% steam, and activity drops to 96% or so
And maintain 12 h constant, steam is turned off rear activity and improved to 98% NO removal efficiencies.
Embodiment ten：1 g aluminium wire nettings are placed in the hydrothermal reaction kettle containing deionized water, 100o12 h of C hydro-thermals.Go from
Sub- water washing 3 times, 100oC dries 12 h, and the boehmite composite material of aluminium wire netting structuring is made.It weighs containing 0.1 g
The cobalt nitrate of the ferric nitrate of Fe and 0.03 g Co are dissolved in 0.8 g methanol, add in 0.26 g zirconium ester coupling agents（ZCA-
N44）, ultrasound 10 minutes.Then it is small to be stood 2 in above-mentioned mixed solution for the boehmite incipient wetness impregnation of aluminium wire netting structuring
Shi Hou instills 0.08 g deionized waters, and standing 4 h makes coupling agent that abundant water occur with the boehmite on monolithic substrate
Solution.Resulting materials 100oC dries 12 h, 500 oCThe iron cobalt for roasting the zirconium dioxide package that aluminium wire netting structuring is made in 3 h is urged
Agent.
The catalytic activity of above-mentioned catalyst is tested, simulated flue gas is by N2、O2、NO、NH3、SO2Composition, wherein NO, NH3、SO2
Volumetric concentration is 500 ppm, O2A concentration of 3%, Balance Air is nitrogen.0.5 g is taken to be put into fixation the catalyst for preparing completion
Active testing is carried out in bed quartz tube reactor, in reaction temperature 90 ~ 510oC, air speed are 20000 h-1Under conditions of,
270-360 oMore than 90% NO removal efficiencies, and N can be achieved between C2Selectivity is 100%.The catalyst is 270oC、SO2
During a concentration of 500 ppm, NO conversion ratios are 99%, and 24 h activity are basically unchanged, and are passed through 10% steam, and activity drops to 97% or so
And maintain 12 h constant, steam is turned off rear activity and improved to 99% NO removal efficiencies.
Embodiment 11：1 g nickel foams are placed in the hydrothermal reaction kettle containing deionized water, add in the nitric acid of 0.01 M
The ammonium chloride of nickel and 0.04 M, 100o3 h of C hydro-thermals.Deionized water washing 3 times, 100oC dries 12 h, and nickel foam structure is made
The nickel hydroxide composite material of change.The cerous nitrate for weighing ferric nitrate and 0.03 g Ce containing 0.1 g Fe is dissolved in 0.8 g methanol
In, add in 0.26 g zirconium ester coupling agents（ZCA-N44）, ultrasound 10 minutes.It then will be at the beginning of the nickel hydroxide of nickel foam structuring
Wet impregnation after standing 2 hours, instills 0.08 g deionized waters, standing 4 h makes coupling agent be carried with monoblock type in above-mentioned mixed solution
The hydroxyl of Strong oxdiative nickel on body is fully hydrolyzed.Resulting materials 100oC dries 12 h, 500 oCIt roasts 3 h and foam is made
The iron cerium catalyst of the zirconium dioxide package of nickel structuring.
The catalytic activity of above-mentioned catalyst is tested, simulated flue gas is by N2、O2、NO、NH3、SO2Composition, wherein NO, NH3、SO2
Volumetric concentration is 500 ppm, O2A concentration of 3%, Balance Air is nitrogen.0.5 g is taken to be put into fixation the catalyst for preparing completion
Active testing is carried out in bed quartz tube reactor, in reaction temperature 90 ~ 510oC, air speed are 20000 h-1Under conditions of,
300-350 oMore than 90% NO removal efficiencies, and N can be achieved between C2 Selectivity is 100%.The catalyst is 270oC、SO2
During a concentration of 500 ppm, NO conversion ratios are 95%, and 24 h activity are basically unchanged, and are passed through 10% steam, and activity drops to 92% or so
And maintain 12 h constant, steam is turned off rear activity and improved to 95% NO removal efficiencies.
Embodiment 12：1 g nickel foams are placed in the hydrothermal reaction kettle containing deionized water, add in the nitric acid of 0.01 M
The ammonium chloride of nickel and 0.04 M, 100o3 h of C hydro-thermals.Deionized water washing 3 times, 100oC dries 12 h, and nickel foam structure is made
The nickel hydroxide composite material of change.The cerous nitrate for weighing ferric nitrate and 0.03 g Ce containing 0.1 g Fe is dissolved in 0.8 g methanol
In, add in the bis- triethanolamine diisopropyl titanate esters of 0.416 g, ultrasound 10 minutes.Then by the hydroxide of nickel foam structuring
Nickel incipient wetness impregnation after standing 2 hours, instills 0.08 g deionized waters, standing 4 h makes coupling agent and entirety in above-mentioned mixed solution
The hydroxyl of nickel hydroxide on formula carrier is fully hydrolyzed.Resulting materials 100oC dries 12 h, 500 oC3 h are roasted to be made
The iron cerium catalyst of the titanium dioxide package of nickel foam structuring.
The catalytic activity of above-mentioned catalyst is tested, simulated flue gas is by N2、O2、NO、NH3、SO2Composition, wherein NO, NH3、SO2
Volumetric concentration is 500 ppm, O2A concentration of 3%, Balance Air is nitrogen.0.5 g is taken to be put into fixation the catalyst for preparing completion
Active testing is carried out in bed quartz tube reactor, in reaction temperature 90 ~ 510oC, air speed are 20000 h-1Under conditions of,
270-420 oMore than 90% NO removal efficiencies, and N can be achieved between C2 Selectivity is 100%.The catalyst is 270oC、SO2
During a concentration of 500 ppm, NO conversion ratios are 96%, and 24 h activity are basically unchanged, and are passed through 10% steam, and activity drops to 93% or so
And maintain 12 h constant, steam is turned off rear activity and improved to 96% NO removal efficiencies.
It is above-mentioned that exemplary embodiment is illustrated, it should not be construed as limiting the invention.Although it has disclosed
Multiple exemplary embodiments, any one skilled in the art in the technical scope disclosed by the present invention, can be light
The change or replacement being readily conceivable that, should be covered by the protection scope of the present invention.Therefore, use and the above embodiment of the present invention
Identical or approximate step and structure, and the preparation method of obtained other metallic monolith denitrating catalysts and implementation should
Denitrating catalyst prepared by method, within protection scope of the present invention.
Claims (14)
1. the nucleocapsid denitrating catalyst of a kind of metallic monoliths, it is characterised in that the denitrating catalyst is with monoblock type
Metal is carrier, and the main active component of area load and auxiliary agent are core, and metal oxide is the catalyst of the nucleocapsid of shell,
The grain size of active component and auxiliary agent is 1~30 nm；The auxiliary agent and the mass ratio of main active component are 0~0.01；Described
The mass ratio of core and shell is 0.1~10.
2. the nucleocapsid denitrating catalyst of metallic monoliths according to claim 1, it is characterised in that above-mentioned whole
Body formula metallic carrier for aluminium, iron, magnesium, nickel, copper, zinc or containing aluminium, iron, magnesium, nickel, copper, zinc alloy woven wire or gold
Belong to foam.
3. the nucleocapsid denitrating catalyst of metallic monoliths according to claim 1, it is characterised in that described
Main active component is one kind of Fe, Mn, Ce.
4. the nucleocapsid denitrating catalyst of metallic monoliths according to claim 1, it is characterised in that described
Auxiliary agent is at least one of manganese, lanthanum, indium, cobalt, copper, nickel, cerium, tungsten, zirconium, vanadium.
5. the nucleocapsid denitrating catalyst of metallic monoliths according to claim 1, it is characterised in that described
Metal oxide is SiO2、Al2O3、TiO2、ZrO2At least one.
6. a kind of nucleocapsid denitration catalyst for preparing metallic monoliths according to any one of claims 1 to 5
The method of agent, it is characterised in that this method the specific steps are：
A. metallic monolith carrier is subjected to hydro-thermal reaction, its surface in situ is made to grow one layer of metal hydroxides；
B. main active component precursor salt, auxiliary agent precursor salt and coupling agent are dissolved in by the mass ratio of 0.1-10 in organic solution, filled
Divide and be uniformly mixed, the coupling agent Ao that homogeneous transparent is made closes solution；
C. by step a obtained by product, be impregnated in coupling agent Ao obtained by step b and close in solution, stand 0.5~4 h, instill
Deionized water, standing 0.5 ~ 5 h makes coupling agent be fully hydrolyzed with the hydroxyl in the hydroxide on monolithic substrate, dries
Afterwards, the catalyst with core-casing structure of metallic monoliths is made in 300-600 DEG C of roasting temperature 3-5 h.
7. the preparation method of the nucleocapsid denitrating catalyst of the metallic monoliths according to claims 6, special
Sign is that the main active component precursor salt is molysite, manganese salt or cerium salt.
8. the preparation method of the nucleocapsid denitrating catalyst of the metallic monoliths according to claims 7, special
Sign is that the molysite is iron chloride, ferric acetate, ferric nitrate or ferric acetyl acetonade；The manganese salt for manganese chloride, manganese acetate,
Manganese nitrate or manganese acetylacetonate；The cerium salt is cerous acetate, cerous nitrate or cerium chloride；Main active constituent is relative to metal entirety
The load capacity of formula carrier is 0.01-30 wt%.
9. the preparation method of the nucleocapsid denitrating catalyst of the metallic monoliths according to claims 6, special
Sign is the auxiliary agent precursor salt in manganese salt, lanthanum salt, indium salts, cobalt salt, mantoquita, nickel salt, cerium salt, tungsten salt, zirconates, vanadic salts
It is at least one.
10. the nucleocapsid denitrating catalyst of the metallic monoliths according to claims 9, it is characterised in that described
Manganese salt be manganese chloride, manganese acetate, one kind in manganese nitrate；Lanthanum salt is lanthanum acetate, one kind of lanthanum nitrate, lanthanum chloride；Indium salts are
Indium acetate, indium nitrate, inidum chloride one kind；Cobalt salt is cobalt chloride, one kind in cobalt acetate, cobalt nitrate；Mantoquita is copper chloride, vinegar
One kind in sour copper, copper nitrate；Nickel salt is nickel chloride, one kind in nickel acetate, nickel nitrate；Cerium salt is cerous acetate, cerous nitrate, chlorine
Change one kind in cerium；Tungsten salt is ammonium tungstate, one kind in ammonium metatungstate, phosphotungstic acid；Zirconates is zirconium nitrate, zirconium sulfate, oxychlorination
One kind in zirconium；Vanadic salts is ammonium metavanadate；Auxiliary agent is 0-30 wt% relative to the load capacity of metallic monolith carrier.
11. the nucleocapsid denitrating catalyst of the metallic monoliths according to claims 6, it is characterised in that described
Coupling agent for esters of silicon acis coupling agent, aluminate coupling agent, titanate coupling agent, zirconium ester coupling agent one kind, shell oxidation
Object is 0-50 wt% relative to the load capacity of metallic monolith carrier.
12. the preparation method of the nucleocapsid denitrating catalyst of the metallic monoliths according to claims 6, special
Sign is that the temperature of the hydro-thermal reaction is 60~180oC, hydro-thermal time are 1~36 h.
13. the preparation method of the nucleocapsid denitrating catalyst of the metallic monoliths according to claims 6, special
Sign is the organic solvent for one kind in methanol, acetone, ethyl alcohol.
14. the preparation method of the nucleocapsid denitrating catalyst of the metallic monoliths according to claims 6, special
Sign is that the dosage of the deionized water is 10~50 wt% of metallic monolith carrier quality.
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