CN100360223C - Sulfur-containing gas catalytic incineration catalyst, preparation method and application - Google Patents
Sulfur-containing gas catalytic incineration catalyst, preparation method and application Download PDFInfo
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- CN100360223C CN100360223C CNB2004100507332A CN200410050733A CN100360223C CN 100360223 C CN100360223 C CN 100360223C CN B2004100507332 A CNB2004100507332 A CN B2004100507332A CN 200410050733 A CN200410050733 A CN 200410050733A CN 100360223 C CN100360223 C CN 100360223C
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- 239000003054 catalyst Substances 0.000 title claims abstract description 69
- 238000002360 preparation method Methods 0.000 title claims abstract description 11
- 230000003197 catalytic effect Effects 0.000 title claims description 28
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 title abstract description 17
- 229910052717 sulfur Inorganic materials 0.000 title abstract description 14
- 239000011593 sulfur Substances 0.000 title abstract description 14
- QGJOPFRUJISHPQ-UHFFFAOYSA-N Carbon disulfide Chemical compound S=C=S QGJOPFRUJISHPQ-UHFFFAOYSA-N 0.000 claims abstract description 48
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical group O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims abstract description 46
- 239000007789 gas Substances 0.000 claims abstract description 36
- 229910052720 vanadium Inorganic materials 0.000 claims abstract description 33
- 150000001875 compounds Chemical class 0.000 claims abstract description 28
- GPPXJZIENCGNKB-UHFFFAOYSA-N vanadium Chemical compound [V]#[V] GPPXJZIENCGNKB-UHFFFAOYSA-N 0.000 claims abstract description 24
- 239000000377 silicon dioxide Substances 0.000 claims abstract description 22
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 16
- 229910001868 water Inorganic materials 0.000 claims abstract description 15
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 claims description 18
- 238000004519 manufacturing process Methods 0.000 claims description 15
- 238000000034 method Methods 0.000 claims description 13
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 claims description 12
- 229910010413 TiO 2 Inorganic materials 0.000 claims description 9
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 8
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 claims description 8
- JMXKSZRRTHPKDL-UHFFFAOYSA-N titanium ethoxide Chemical compound [Ti+4].CC[O-].CC[O-].CC[O-].CC[O-] JMXKSZRRTHPKDL-UHFFFAOYSA-N 0.000 claims description 8
- 238000001035 drying Methods 0.000 claims description 6
- 235000006408 oxalic acid Nutrition 0.000 claims description 6
- 150000003609 titanium compounds Chemical class 0.000 claims description 6
- UNTBPXHCXVWYOI-UHFFFAOYSA-O azanium;oxido(dioxo)vanadium Chemical compound [NH4+].[O-][V](=O)=O UNTBPXHCXVWYOI-UHFFFAOYSA-O 0.000 claims description 5
- FPCJKVGGYOAWIZ-UHFFFAOYSA-N butan-1-ol;titanium Chemical compound [Ti].CCCCO.CCCCO.CCCCO.CCCCO FPCJKVGGYOAWIZ-UHFFFAOYSA-N 0.000 claims description 5
- 229910052739 hydrogen Inorganic materials 0.000 claims description 5
- 239000001257 hydrogen Substances 0.000 claims description 5
- VXUYXOFXAQZZMF-UHFFFAOYSA-N titanium(IV) isopropoxide Chemical compound CC(C)O[Ti](OC(C)C)(OC(C)C)OC(C)C VXUYXOFXAQZZMF-UHFFFAOYSA-N 0.000 claims description 5
- 238000005470 impregnation Methods 0.000 claims description 4
- 239000003960 organic solvent Substances 0.000 claims description 4
- 239000011148 porous material Substances 0.000 claims description 4
- -1 sulfide hydrogen Chemical class 0.000 claims description 4
- YONPGGFAJWQGJC-UHFFFAOYSA-K titanium(iii) chloride Chemical compound Cl[Ti](Cl)Cl YONPGGFAJWQGJC-UHFFFAOYSA-K 0.000 claims description 4
- 238000007598 dipping method Methods 0.000 claims description 3
- LXASOGUHMSNFCR-UHFFFAOYSA-D [V+5].[V+5].[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O Chemical compound [V+5].[V+5].[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O LXASOGUHMSNFCR-UHFFFAOYSA-D 0.000 claims description 2
- 229910052799 carbon Inorganic materials 0.000 claims description 2
- 238000007654 immersion Methods 0.000 claims description 2
- 238000005245 sintering Methods 0.000 claims description 2
- UUUGYDOQQLOJQA-UHFFFAOYSA-L vanadyl sulfate Chemical compound [V+2]=O.[O-]S([O-])(=O)=O UUUGYDOQQLOJQA-UHFFFAOYSA-L 0.000 claims description 2
- RAHZWNYVWXNFOC-UHFFFAOYSA-N Sulphur dioxide Chemical compound O=S=O RAHZWNYVWXNFOC-UHFFFAOYSA-N 0.000 abstract description 59
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 abstract description 33
- 229910000037 hydrogen sulfide Inorganic materials 0.000 abstract description 33
- 238000006243 chemical reaction Methods 0.000 abstract description 26
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 abstract description 13
- 239000010936 titanium Substances 0.000 abstract description 11
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 abstract description 6
- 230000000694 effects Effects 0.000 abstract description 6
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 abstract description 4
- 229910052719 titanium Inorganic materials 0.000 abstract description 4
- 229910002092 carbon dioxide Inorganic materials 0.000 abstract description 3
- 239000001569 carbon dioxide Substances 0.000 abstract description 3
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 abstract description 3
- 238000005670 sulfation reaction Methods 0.000 abstract description 3
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 abstract description 3
- 230000019635 sulfation Effects 0.000 abstract description 2
- JJWKPURADFRFRB-UHFFFAOYSA-N carbonyl sulfide Chemical compound O=C=S JJWKPURADFRFRB-UHFFFAOYSA-N 0.000 abstract 4
- 235000012239 silicon dioxide Nutrition 0.000 abstract 2
- XHCLAFWTIXFWPH-UHFFFAOYSA-N [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] XHCLAFWTIXFWPH-UHFFFAOYSA-N 0.000 abstract 1
- 229910001935 vanadium oxide Inorganic materials 0.000 abstract 1
- 235000010269 sulphur dioxide Nutrition 0.000 description 28
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 11
- 230000003647 oxidation Effects 0.000 description 11
- 238000007254 oxidation reaction Methods 0.000 description 11
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 8
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 description 8
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 8
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 6
- 238000005516 engineering process Methods 0.000 description 6
- 238000011156 evaluation Methods 0.000 description 6
- XDAHMMVFVQFOIY-UHFFFAOYSA-N methanedithione;sulfane Chemical compound S.S=C=S XDAHMMVFVQFOIY-UHFFFAOYSA-N 0.000 description 6
- 239000000203 mixture Substances 0.000 description 6
- 239000004408 titanium dioxide Substances 0.000 description 6
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 5
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 4
- 229910052797 bismuth Inorganic materials 0.000 description 4
- QGJOPFRUJISHPQ-NJFSPNSNSA-N carbon disulfide-14c Chemical compound S=[14C]=S QGJOPFRUJISHPQ-NJFSPNSNSA-N 0.000 description 4
- 229910052751 metal Inorganic materials 0.000 description 4
- 239000002184 metal Substances 0.000 description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- 229910052697 platinum Inorganic materials 0.000 description 4
- 238000011084 recovery Methods 0.000 description 4
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 3
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 description 3
- 239000005864 Sulphur Substances 0.000 description 3
- JCXGWMGPZLAOME-UHFFFAOYSA-N bismuth atom Chemical compound [Bi] JCXGWMGPZLAOME-UHFFFAOYSA-N 0.000 description 3
- 229910052742 iron Inorganic materials 0.000 description 3
- 229910052750 molybdenum Inorganic materials 0.000 description 3
- 239000011733 molybdenum Substances 0.000 description 3
- 125000001741 organic sulfur group Chemical group 0.000 description 3
- 229910052763 palladium Inorganic materials 0.000 description 3
- 239000002912 waste gas Substances 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 2
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 2
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 2
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 2
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 2
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 229910002091 carbon monoxide Inorganic materials 0.000 description 2
- 229910052804 chromium Inorganic materials 0.000 description 2
- 239000011651 chromium Substances 0.000 description 2
- 229910017052 cobalt Inorganic materials 0.000 description 2
- 239000010941 cobalt Substances 0.000 description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 239000003205 fragrance Substances 0.000 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 description 2
- 229910052680 mordenite Inorganic materials 0.000 description 2
- 229910052759 nickel Inorganic materials 0.000 description 2
- 229910000510 noble metal Inorganic materials 0.000 description 2
- 150000002898 organic sulfur compounds Chemical class 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 238000006213 oxygenation reaction Methods 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- 239000000741 silica gel Substances 0.000 description 2
- 229910002027 silica gel Inorganic materials 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- 229910052718 tin Inorganic materials 0.000 description 2
- 239000011135 tin Substances 0.000 description 2
- 230000001988 toxicity Effects 0.000 description 2
- 231100000419 toxicity Toxicity 0.000 description 2
- RBORURQQJIQWBS-QVRNUERCSA-N (4ar,6r,7r,7as)-6-(6-amino-8-bromopurin-9-yl)-2-hydroxy-2-sulfanylidene-4a,6,7,7a-tetrahydro-4h-furo[3,2-d][1,3,2]dioxaphosphinin-7-ol Chemical compound C([C@H]1O2)OP(O)(=S)O[C@H]1[C@@H](O)[C@@H]2N1C(N=CN=C2N)=C2N=C1Br RBORURQQJIQWBS-QVRNUERCSA-N 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 230000010718 Oxidation Activity Effects 0.000 description 1
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 description 1
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- 229910021536 Zeolite Inorganic materials 0.000 description 1
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 1
- 238000010306 acid treatment Methods 0.000 description 1
- 239000004411 aluminium Substances 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 229910052787 antimony Inorganic materials 0.000 description 1
- WATWJIUSRGPENY-UHFFFAOYSA-N antimony atom Chemical compound [Sb] WATWJIUSRGPENY-UHFFFAOYSA-N 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 229910052793 cadmium Inorganic materials 0.000 description 1
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 description 1
- 239000004568 cement Substances 0.000 description 1
- 239000000567 combustion gas Substances 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 1
- 239000012153 distilled water Substances 0.000 description 1
- 238000004134 energy conservation Methods 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000005755 formation reaction Methods 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 238000005984 hydrogenation reaction Methods 0.000 description 1
- 229910052741 iridium Inorganic materials 0.000 description 1
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 1
- RUTXIHLAWFEWGM-UHFFFAOYSA-H iron(3+) sulfate Chemical compound [Fe+3].[Fe+3].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O RUTXIHLAWFEWGM-UHFFFAOYSA-H 0.000 description 1
- 229910000360 iron(III) sulfate Inorganic materials 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- 238000012423 maintenance Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 239000003345 natural gas Substances 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 239000011574 phosphorus Substances 0.000 description 1
- 229910052698 phosphorus Inorganic materials 0.000 description 1
- 231100000572 poisoning Toxicity 0.000 description 1
- 230000000607 poisoning effect Effects 0.000 description 1
- 229910052700 potassium Inorganic materials 0.000 description 1
- 239000011591 potassium Substances 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 238000007670 refining Methods 0.000 description 1
- 229910052703 rhodium Inorganic materials 0.000 description 1
- 239000010948 rhodium Substances 0.000 description 1
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 1
- 239000010865 sewage Substances 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- 238000004148 unit process Methods 0.000 description 1
- 238000005303 weighing Methods 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 description 1
- 239000010457 zeolite Substances 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
- 239000011701 zinc Substances 0.000 description 1
Landscapes
- Catalysts (AREA)
- Exhaust Gas Treatment By Means Of Catalyst (AREA)
Abstract
本发明提供了含硫气体焚烧催化剂及其制备方法，催化剂载体为二氧化硅，活性组分为钒和钛的氧化物。以催化剂重量计：二氧化硅的含量为65%～95%，钒的氧化物含量为0.5%～15%，钛的氧化物含量为0.5%～20%。本发明的催化剂活性高、耐硫酸盐化，可用于气体中的硫化氢、二硫化碳和羰基硫等化合物的焚烧处理，将上述化合物氧化为二氧化硫、二氧化碳和水。催化剂的操作温度为200～400℃，空速为2000～10000h-1。催化剂操作温度300℃、空速5000h-1时，硫化氢的转化率高于99%，二硫化碳和羰基硫的转化率高于85%，二氧化硫生成率高于96%。The invention provides a sulfur-containing gas burning catalyst and a preparation method thereof. The catalyst carrier is silicon dioxide, and the active components are oxides of vanadium and titanium. Based on the weight of the catalyst: the content of silicon dioxide is 65%-95%, the content of vanadium oxide is 0.5%-15%, and the content of titanium oxide is 0.5%-20%. The catalyst of the invention has high activity and resistance to sulfation, and can be used for incineration treatment of compounds such as hydrogen sulfide, carbon disulfide and carbonyl sulfide in gas, and oxidizes the above compounds into sulfur dioxide, carbon dioxide and water. The operating temperature of the catalyst is 200-400°C, and the space velocity is 2000-10000h -1 . When the catalyst operating temperature is 300°C and the space velocity is 5000h -1 , the conversion rate of hydrogen sulfide is higher than 99%, the conversion rate of carbon disulfide and carbonyl sulfide is higher than 85%, and the generation rate of sulfur dioxide is higher than 96%.
Description
Technical field
The present invention relates to sulfurous gas catalyst to burned and its production and application, be applicable to the exhaust-gas treatment of compounds such as all kinds of sulfide hydrogens, carbon disulfide and cos, above-mentioned sulfide can be converted into stink and all lower sulfur dioxide of toxicity, the catalytic burning that is specially adapted to sulfur recovery claus process tail gas, geothermal power plant's waste gas is handled.
Background technology
Hydrogen sulfide and organic sulfur compound (as carbon disulfide, cos) are that a class has the odorant pollutant of toxicity in various degree to human body, mainly from industrial tail gas such as oil refining, natural gas, chemical industry, sewage disposal, geothermal power generations.With the oil plant is example, contains a certain amount of hydrogen sulfide and organic sulfur compound in its sulfur recovery tail gas, for satisfying the odorant pollutant discharge standard, could discharge after must burning.Because the combustible component (as hydrogen sulfide, cos, carbon monoxide, carbon disulfide, hydrogen, elementary sulfur and a small amount of oil gas) in the tail gas often is lower than 3% of tail gas total amount, must postcombustion, could completing combustion, and be sulfur dioxide with sulfide oxidation.The tail gas burning process has thermal incineration and catalytic burning two classes.The thermal incineration method is carried out excessive oxygen and 700～820 ℃ usually.Owing to be difficult to accurately control operating conditions such as incineration temperature, the situation that incinerator crumples often appears in the practice, reduced the service life of incinerator.Catalytic burning can make hydrogen sulfide, carbon disulfide and cos in the tail gas be oxidized to sulfur dioxide with lower temperature (as 300～400 ℃) under catalyst action.The output investment ratio thermal incineration of catalytic burning is high approximately by 10%, and energy consumption and operating cost can save nearly 50%.The actual gain of catalytic burning is relevant with the scale of device, and the sulfur recovery unit of a 100t/d can be saved 1000m
3The combustion gas of/d, the fuel cost of catalyst length of life saving are more than 10 times of institute's spent catalyst expense.Therefore, catalytic burning can satisfy environmental protection and energy-conservation needs simultaneously.
Catalyst is the pith of sulfurous gas catalytic burning technology, and the key of this class catalyst performance is how to overcome the sulfation of catalyst active center, the stability of the long-time running of maintenance catalyst and active.CN1049299A discloses a kind of sulfur-bearing organic catalyst to burned waste gas and preparation method thereof, and this catalyst is a carrier with the natural mordenite zeolite of sulfuric acid treatment modification, V
2O
5Be main active component, noble metals such as a spot of platinum, palladium are the auxiliary activity component, V
2O
5Content is 0.4%～0.7% (mass percent, down with), and platinum content is 0.01%～0.02%, and palladium content is 0.02%～0.03%, also can contain one or more of 0.01%～0.07% cobalt, manganese, molybdenum, nickel, potassium, na oxide.At 320～380 ℃ of reaction temperatures, air speed 4800～10000h
-1, during organic sulfur concentration 800～10000mg/l, conversion ratio 〉=99%.This catalyst loading noble metal, cost is higher, sulfur poisoning-resistant is limited in one's ability.CN1410149A discloses catalyst to burned and the preparation and the using method of hydrogen sulfide in a kind of gas, and the carrier of this catalyst is a silica, and active component is the oxide of iron and vanadium.This invention is applicable to hydrogen sulfide, oxidation activity the unknown of organic sulfur.CN1163785A discloses the catalytic burning technique of hydrogen sulfide in a kind of gas, is suitable for handling Claus tail gases, and with the active carbon catalyst, be under 200～400 ℃ in temperature, be sulfur dioxide with the hydrogen sulfide catalytic oxidation.Hydrogen sulfide content is 0.5%～4% (v/v), moisture content 4%～30% (v/v), air speed 3000～10000h
-1, the conversion ratio of hydrogen sulfide is 100%, sulfur dioxide production rate 90%～99%.USP4576184,4444908,4528277,4444741,4444742,4314983 disclose a class hydrogen sulfide oxidation catalyst and a technology, this activity of such catalysts component comprises vanadium and bismuth, also can constitute by vanadium and tin or antimony, carrier is the porous refractory oxide, by aluminium oxide, silica-alumina, silica, titanium dioxide, zirconia, silica-titania, silica-zirconia, one or more formations in silica-zirconia-titanium dioxide, hydrogen sulfide can be oxidized to sulphur or sulfur dioxide, characteristics are when steam exists, and still have high activity and stability.For example active component is 11.6%Bi
2O
3+ 8.6%V
2O
5Catalyst, at 240 ℃ of reaction temperatures, air speed 2000h
-1, the hydrogen sulfide of 2717ppm is converted into sulfur dioxide fully, and hydrogen and methane are not oxidized.USP4427576,4937058 disclose a kind of catalyst and preparation technology thereof who hydrogen sulfide or organic sulfur is oxidized to sulfur dioxide, the carrier of this catalyst is a titanium dioxide, or the mixture of titanium dioxide and zirconia or silica, active component is made of at least a of a kind of alkali earth metal sulfate and following metal: copper, silver, zinc, cadmium, yttrium, lanthanum, vanadium, chromium, molybdenum, tungsten, manganese, iron, cobalt, rhodium, iridium, nickel, palladium, platinum, tin and bismuth, the content of carrier is 60%～99%, the content of alkali earth metal sulfate is 1%～40%, and the specific surface of catalyst is 20～500m
2/ g.380 ℃ of reaction temperatures, air speed 1800h
-1Feeding gas sulfide hydrogen 800ppm, cos 100ppm, carbon disulfide 500ppm, sulfur dioxide 400ppm, oxygen 2%, steam 30%, nitrogen 67.82%, the catalytic conversion of hydrogen sulfide＞99%, the catalytic conversion 61%～98% of carbon disulfide, the catalytic conversion 52%～94% of cos.USP4148760 discloses a kind of selective oxidation of sulfur containing compounds in particular catalyst, and its carrier is an alumina cement, and active component is V
2O
5And Fe
2O
3, also can contain titanium and silver-colored oxide.This catalyst can be oxidized to sulfur dioxide with the hydrogen sulfide in the Claus tail gases, cos, carbon disulfide.USP4197277 discloses a kind of selective oxidation of sulfur containing compounds in particular catalyst, and its carrier is an aluminium oxide, and active component is V
2O
5And Fe
2O
3, also can contain titanium and silver-colored oxide.This catalyst can be oxidized to sulfur dioxide with the hydrogen sulfide in the Claus tail gases, cos, carbon disulfide.It can be the catalyst of sulfur dioxide with selective oxidation of sulfur containing compounds in particular that USP5278123 discloses a kind of, and carrier is a titanium dioxide, and active component is iron and platinum.USP6019953 discloses a kind of gas burning process, is applicable to the catalytic burning of sulphide-rich gas.First metal component of catalyst is bismuth, molybdenum or chromium, and second metal component is one or more of Group IIA metal, and carrier is a refractory oxide, can not contain aluminium and phosphorus simultaneously in the carrier.The hydrogen sulfide complete oxidation temperature that example provides is 500 ℃.USP4169136,4092404,4171347,4088743 discloses the catalytic burning technique of hydrogen sulfide in the class gas, this technology can be oxidized to sulfur dioxide with hydrogen sulfide, operating temperature is 150～480 ℃, the activity of such catalysts component is the oxide of vanadium and/or the sulfide of vanadium, and carrier is non-alkaline porous refractory oxide.A kind of well behaved catalyst is 5%～15% V
2O
5/ hydrogenation mordenite or aluminium oxide.Hydrogen in the feeding gas, carbon monoxide, lighter hydrocarbons and ammonia are not oxidized, and patent has been used for geothermal power plant's treatment of waste gas.USP4399112 discloses a kind of sulphur-containing exhaust gas catalytic burning technique, can be used for the processing of Claus tail gases, this technology has two stages to constitute, be hydrogen sulfide at first with carbon disulfide, cos, mercaptan sulfides hydrogenating reduction, and then be sulfur dioxide with the hydrogen sulfide catalytic oxidation, the catalyst of its oxidation panel is ferric sulfate/titanium dioxide.
Summary of the invention
Sulfurous gas catalyst to burned that the invention provides a kind of active height, good stability and preparation method thereof reaches Application of Catalyst.
Sulfurous gas catalyst to burned of the present invention is a carrier with silica, is active component with vanadium and titanyl compound.In catalyst weight: the content of silica is 65%～95%, and the oxide content of vanadium is 0.5%～15%, and is preferred 1%～8%, and titanyl compound content is 0.5%～20%, is preferably 2%～10%.The specific area of catalyst is 200～350m
2/ g, pore volume are 0.3～0.8ml/g.
Catalyst of the present invention can be used for the burning disposal of one or more sulfur-containing compounds in hydrogen sulfide, carbon disulfide and the cos etc. in the gas, is sulfur dioxide, carbon dioxide and water with above-mentioned selective oxidation of sulfur containing compounds in particular.
The thing of silica supports is amorphous phase mutually, can select water-fast gross porosity spherical silica gel for use, and its specific area is 200～400m
2/ g, pore volume are 0.4～0.9ml/g.The oxide of vanadium is V
2O
5, titanyl compound is TiO
2
The optimum shape of catalyst of the present invention is 4～6mm sphere, can adopt immersion process for preparing, and two kinds of preparation procedures are arranged, and is as follows:
(1) use organic titanic compound (as isopropyl titanate Ti (OCH (CH earlier
3)
2)
4, butyl titanate Ti (OC
4H
9)
4, tetraethyl titanate Ti (OC
2H
5)
4Deng) organic solution (as toluene, ethanol or isopropyl alcohol etc.) or the ethanolic solution impregnation of silica carrier (through 120 ℃ of oven dry) of titanium trichloride, with the organic solvent evaporated in vacuo, after gained sample drying, the roasting, use the oxalic acid solution dipping of the water soluble compound of vanadium again, dry then, roasting, titanium compound is decomposed into TiO through roasting
2, the water soluble compound of vanadium is decomposed into V through roasting
2O
5The water soluble compound of vanadium is one or more in ammonium metavanadate, vanadic sulfate, the vanadium oxalate, and the water soluble compound of vanadium is preferably ammonium metavanadate, and the water soluble compound of vanadium is dissolved in the oxalic acid solution of 1.0～2.0mol/L.The water soluble compound of titanium is preferably butyl titanate.
(2) elder generation after drying, the roasting, uses organic titanic compound (as isopropyl titanate Ti (OCH (CH with the oxalic acid solution impregnation of silica carrier (through 120 ℃ of oven dry) of the water soluble compound (as ammonium metavanadate) of vanadium again
3)
2)
4, butyl titanate Ti (OC
4H
9)
4, tetraethyl titanate Ti (OC
2H
5)
4Deng) organic solution (as toluene, ethanol or isopropyl alcohol etc.) or the ethanolic solution of titanium trichloride dipping, with the organic solvent evaporated in vacuo, dry then, roasting.Titanium compound is decomposed into TiO through roasting
2, the water soluble compound of vanadium is decomposed into V through roasting
2O
5
Baking temperature is generally 110～150 ℃ in the above-mentioned preparation process, and be 2～12h drying time, and sintering temperature is 450～550 ℃, and roasting time is 4～5h.
Catalyst of the present invention is used for the catalytic burning of sulfurous gas (as hydrogen sulfide, carbon disulfide, cos etc.), is specially adapted to the catalytic burning of oil plant Sulfur Recovery Unit process tail gas.Its technical process is: sulfurous gas is mixed with excess air, after the preheating, with 2000～10000h
-1Air speed by the catalytic burning stove, under 200～400 ℃ of reaction temperatures, hydrogen sulfide, carbon disulfide and cos are sulfur dioxide, carbon dioxide and water by catalytic oxidation.
Owing to have the effect of influencing each other between each component of catalyst, have different serviceabilities so different components cooperates.The characteristics of catalyst of the present invention are: the catalytic activity height, and under optimum condition, the oxygenation efficiency of hydrogen sulfide is higher than 99%, and the oxygenation efficiency of carbon disulfide and cos is higher than 85%, and the sulfur dioxide production rate is higher than 96%; Catalyst life is longer, all anti-sulfation of carrier and active component; 200～400 ℃ of operating temperatures, empty scooter 10000h
-1
The specific embodiment
Embodiment 1
Take by weighing isopropyl titanate [Ti (OCH (CH
3)
2)
4] 18.4g is dissolved in the 100ml toluene, to be dipped in wherein through the water-fast gross porosity spherical silica gel of the 4～6mm 100g of 120 ℃ of oven dry 2h and stir evenly, leave standstill 12h, then under 60 ℃ with rotary evaporator with the solvent evaporate to dryness, at 120 ℃ of dry 6h, next 500 ℃ of roasting 4h in air immerse by 7.1g ammonium metavanadate, 25.2g oxalic acid (C
2H
2O
42H
2O) and in the solution formed of 100ml distilled water, after stirring evenly under 30 ℃, leave standstill 12h, then under 50 ℃ with rotary evaporator with the water evaporate to dryness, behind 120 ℃ of dry 6h, 500 ℃ of roasting 4h obtain catalyst sample in air.This catalyst consists of: silica 90%, V
2O
55%, TiO
25%.On small-sized catalytic burning experimental rig, this catalyst to be estimated, feed composition is hydrogen sulfide 1% (v/v), carbon disulfide 0.1% (v/v), cos 0.1% (v/v), steam 30% (v/v), 300 ℃ of reaction temperatures, air speed 5000h
-1Evaluation result sees Table 1.
The conversion ratio of table 1 sulfide and the production rate of sulfur dioxide
| Hydrogen sulfide | Carbon disulfide | Cos | |
| Conversion ratio, % | 100 | 85 | 88 |
| The sulfur dioxide production rate, % | 100 | 96 | 98 |
Embodiment 2
Catalyst consists of: silica 85%, V
2O
55%, TiO
210%.Feed composition is hydrogen sulfide 1% (v/v), carbon disulfide 0.1% (v/v), cos 0.1% (v/v), steam 30% (v/v).300 ℃ of reaction temperatures, air speed 5000h
-1Evaluation result sees Table 2.
The conversion ratio of table 2 sulfide and the production rate of sulfur dioxide
| Hydrogen sulfide | Carbon disulfide | Cos | |
| Conversion ratio, % | 100 | 88 | 90 |
| The sulfur dioxide production rate, % | 100 | 98 | 99 |
Embodiment 3
Catalyst consists of: silica 90%, V
2O
55%, TiO
25%.Feed composition is hydrogen sulfide 1% (v/v), carbon disulfide 0.1% (v/v), cos 0.1% (v/v), steam 30% (v/v).300 ℃ of reaction temperatures, air speed 10000h
-1Evaluation result sees Table 3.
The conversion ratio of table 3 sulfide and the production rate of sulfur dioxide
| Hydrogen sulfide | Carbon disulfide | Cos | |
| Conversion ratio, % | 99 | 75 | 80 |
| The sulfur dioxide production rate, % | 100 | 95 | 96 |
Embodiment 4
Catalyst consists of: silica 90%, V
2O
55%, TiO
25%.Feed composition is hydrogen sulfide 1% (v/v), carbon disulfide 0.1% (v/v), cos 0.1% (v/v), steam 30% (v/v).350 ℃ of reaction temperatures, air speed 5000h
-1Evaluation result sees Table 4.
The conversion ratio of table 4 sulfide and the production rate of sulfur dioxide
| Hydrogen sulfide | Carbon disulfide | Cos | |
| Conversion ratio, % | 100 | 88 | 92 |
| The sulfur dioxide production rate, % | 100 | 98 | 99 |
Embodiment 5
Catalyst consists of: silica 80%, V
2O
510%, TiO
210%.
Embodiment 6
Catalyst consists of: silica 85%, V
2O
510%, TiO
25%.
Embodiment 7
Catalyst consists of: silica 93%, V
2O
52%, TiO
25%.
Embodiment 5～7 described catalyst are used for the catalytic burning of sulphur-containing exhaust gas to be handled.Feed composition is hydrogen sulfide 1% (v/v), carbon disulfide 0.1% (v/v), cos 0.1% (v/v), steam 30% (v/v).350 ℃ of reaction temperatures, air speed 5000h
-1Evaluation result sees Table 5.
Table 5 embodiment 5～7 catalyst application results
| Conversion ratio, %/sulfur dioxide production rate, % | Hydrogen sulfide | Carbon disulfide | Cos |
| Embodiment 5 | 100/100 | 89/99 | 93/99 |
| Embodiment 6 | 100/100 | 88/98 | 92/99 |
| Embodiment 7 | 99/99 | 83/96 | 85/98 |
Comparative example
By the catalyst A that CN1410149A embodiment 1 makes, estimate by the evaluation method of the embodiment of the invention 1, the results are shown in Table 6.
Table 6 comparative example catalyst experiment result
| Hydrogen sulfide | Carbon disulfide | Cos | |
| Conversion ratio, % | 100 | 55 | 70 |
| The sulfur dioxide production rate, % | 99 | 85 | 90 |
Claims (9)
1, a kind of sulfurous gas catalytic incineration catalyst, it is characterized in that with silica being carrier, with vanadium and titanyl compound is active component, in catalyst weight: the content of silica is 65%～95%, the oxide content of vanadium is 0.5%～15%, titanyl compound content is 0.5%～20%, and the specific area of described catalyst is 200～350m
2/ g, pore volume are 0.3～0.8ml/g.
2, according to the described catalyst of claim 1, the oxide content that it is characterized in that described vanadium is 1%～%, and titanyl compound content is 2%～10%.
3, according to the described catalyst of claim 1, it is characterized in that described silica supports is an amorphous phase, its specific area is 200～400m
2/ g, pore volume are 0.4～0.9ml/g; The oxide of vanadium is V
2O
5, titanyl compound is TiO
2
4, according to the described arbitrary Preparation of catalysts method of claim 1 to 3, it is characterized in that adopting immersion process for preparing; With the organic solution impregnation of silica carrier of titanium compound,, after gained sample drying, the roasting, use the oxalic acid solution dipping of the water soluble compound of vanadium again, dry then, roasting earlier with the organic solvent evaporated in vacuo; Or use the oxalic acid solution of the water soluble compound of vanadium to flood earlier, after gained sample drying, the roasting, use the organic solution impregnation of silica carrier of titanium compound again, with organic solvent evaporated in vacuo, roasting then; The organic solution of described titanium compound is toluene, ethanol or the aqueous isopropanol of isopropyl titanate, butyl titanate or tetraethyl titanate, perhaps is the ethanolic solution of titanium trichloride.
5, in accordance with the method for claim 4, it is characterized in that the baking temperature in the catalyst preparation process is 110～150 ℃, be 2～12h drying time, and sintering temperature is 450～550 ℃, and roasting time is 4～5h.
6, in accordance with the method for claim 4, the water soluble compound that it is characterized in that described vanadium is one or more in ammonium metavanadate, vanadic sulfate, the vanadium oxalate; Titanium compound is one or more in titanium trichloride, isopropyl titanate, butyl titanate, the tetraethyl titanate.
7, the application of the arbitrary catalyst of a kind of claim 1 to 3 in the sulfurous gas catalytic burning.
8,, it is characterized in that in described sulfurous gas sulfide hydrogen, carbon disulfide and the cos one or more according to the described application of claim 7.
9,, it is characterized in that the catalytic burning air speed is 2000～10000h according to the described application of claim 7
-1, temperature is 200～400 ℃.
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|---|---|---|---|
| CNB2004100507332A CN100360223C (en) | 2004-10-29 | 2004-10-29 | Sulfur-containing gas catalytic incineration catalyst, preparation method and application |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CNB2004100507332A CN100360223C (en) | 2004-10-29 | 2004-10-29 | Sulfur-containing gas catalytic incineration catalyst, preparation method and application |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN1768928A CN1768928A (en) | 2006-05-10 |
| CN100360223C true CN100360223C (en) | 2008-01-09 |
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|---|---|---|---|
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| TWI781956B (en) * | 2016-10-06 | 2022-11-01 | 丹麥商托普索公司 | A method for cleaning viscose production off-gases and catalysts for use in the method |
| CN113289602A (en) * | 2021-06-01 | 2021-08-24 | 清华大学 | Catalyst for carbonyl sulfide hydrolysis in blast furnace gas and preparation method and application thereof |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4002653A (en) * | 1974-06-26 | 1977-01-11 | Basf Aktiengesellschaft | Manufacture of anthraquinone |
| JPH0295416A (en) * | 1988-09-22 | 1990-04-06 | Haashau Kemi Bv | Removal of nitrogen oxide from flue gas by selective reduction |
| CN1410149A (en) * | 2001-10-08 | 2003-04-16 | 中国石化集团齐鲁石油化工公司 | Combustion catalyst of hydrogen sulfide in gas and its preparation and use method |
-
2004
- 2004-10-29 CN CNB2004100507332A patent/CN100360223C/en not_active Expired - Lifetime
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4002653A (en) * | 1974-06-26 | 1977-01-11 | Basf Aktiengesellschaft | Manufacture of anthraquinone |
| JPH0295416A (en) * | 1988-09-22 | 1990-04-06 | Haashau Kemi Bv | Removal of nitrogen oxide from flue gas by selective reduction |
| CN1410149A (en) * | 2001-10-08 | 2003-04-16 | 中国石化集团齐鲁石油化工公司 | Combustion catalyst of hydrogen sulfide in gas and its preparation and use method |
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