Effect of Additive on Sulfur-fixation Process of Sulfur-fixation Agent Effect of Additive on Sulfur-fixation Process of Sulfur-fixation Agent

Effect of Additive on Sulfur-fixation Process of Sulfur-fixation Agent

  • 期刊名字:武汉理工大学学报英
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  • 论文作者:XIE Jun-lin,QIU Jian-rong,ZHAO
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  • 更新时间:2020-11-11
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论文简介

Vol.18 No.4Jouna of Wuhan Lniversity of Technology - Maler. Sxi. Fd.Dee.2003Effect of Additive on Sulfur-fixationProcess of Sulfur - fixation Agent'06 AXIE Jun- lin'QIU Jian-rongZHAO Gai-ju LOU Jin- ping2HAN Chun-hua”Huazhang University of Science &Techrnology 2) Wuhan University of Technology( Received: Dec. 20, 2002; Accepted: May 10, 2003)Abstract: The rstaliation behaxior o/ desufurioution prducrt is direnly related 10 is high lemyeraurresisant ability . Fjfers of the additive on the slfurfixution ficiencng 0/ the Rat sufur fintions agent and also onthe cpstalization beharior of the sulur; fxudionu prolut were studied when Ca003 and BuC03 vere wserd as thedsufurzution agent and Mg0 and SrCO, lsed as the ssarusts sulfur, fxntion agent . The result shous thut increase of sufur fxation capabiliy ,for the uklire is not oue to their dirctly renct 10 Jorm sufate or intract with(CaCO, and BaCO3 to form cunpusile minerl heut reistant in high tenpernlure, buu onve to their acrintin tosulfur : fxation reasion of the suftr fxatin agentKey words: desufurizution; cstalintion behawior; suf-fuiono1 Introductionrization, the rcaction of Ca0 with SO2 is easy to occur audlform the muliple minerals when compounds of Va, K,The research on the desufurization of the coal withFe, Mn, Sr etc are used as the asistanl agent, which in-creases the rcsolved leunperalure of the CaSO4. Thoughhigh sulfur is always an important topic in the research onthe crystallization behavior of desulfurization produ:t is心the environmental pollution control , the eficient dsulu-rization technology has llraleledl more and more atentionlated directly to its high-temperature- rsistunt capaeity, itof rescarchers in the phase of coal and environment:'2.is not given much rmor: altcntion to the relationship be-The statistics from US Fnvironmental Burau show thattween the erystallization behavior and the resolved teuper-ature in almost all the researches. 'Thcir researthes arethere are almosl 200 kinds o[ methods for the control tech-nologies of S02 in the world, among which the combustionlimited on hole structure CVCn if there are reports on thedesulfurizalion methods are noticed because they noed notstructurc, and the crystallization theory on desufurizatiouproduct is almost blank .the extra desulfuriration equipment, and they are mor:ffeels of the additive on the sulfur- fixation efciceccunonical .Calcium is curently one kind of desufrizatin aganlcy of desulfrization agent and the rysllizalion bchaviorstudied and used more in the world, aurd the theury of itsof sulfur- fixation produet were slutied in this article whendesulfurization lends to be ripe. Desulfurization combus-CaCO3 and BaCO; were used as the desulfurixation agenltion technologies on the fluidized-bed are beginning to beand MgO and SrC03 used as the assistant sulfur-fixationused in large pwwer plants in China. But the sulfur-fixa-agent.tion fficiency of caleium is lower due to the complexity ofthe sulfrfixation process and the re-resolvec of the sul-2 Experimentalphuate al high ternperature. In order to increase the sulfur-Coal with high ash contcnt in Heshan east mine wasfixation fficiency ,an assistant agent is added for the pur-pose of imprv ing the surface activity of the desulfurizationselected as the cxprime'ntal sample , and its industry anal-and increasing the resolved temperature of the desulfuriza-ysis value , element analysis value and cheniral componenttion product CaSO, . Studies .4 show that in the desulfu-of ash are shown in Tablcs 1 and 2. BaCO, (chemical pureis 99%) was seleted as he sulfur- fixation agent, andXIE. Jun-lin(谢峻林): Bom in 1965; Ph D; Prof. ; PosldoctorMgO and SrCO, were used as the astant sufur-fivationof Huazhong University of Science &Technology; Sthool of Energyagent. In order to compare the inpacts of the Ba-sulfur-and Power Fngineeing, Wuhan 430074, China. Enaged in cleanfixation and Ca-sulfur-fixation ,the sulfur-fixation efficien-coal technology of cement industry* Funded by the Nationul Nalural Science Founduation of Chi-中国煤化工) was sudied acond-a (No. 50276045). Daclonl Subjexl Founduliun of China ( No.20010487011 ),and Postdoctor Fourndution uf Chinu ( No.MYHCNMHG0106121002)7ol.18 No.4XIE Junr lin以al : Elect of Additive on Sulfur - fixation Prucess of.5:Table | Results of the Industry Analyis and the Flemcntperature, while increasing the: temperatur: continuouslyAnalysis of the (oalwill make: a part of the crystal in high tempealure resolvelodustry arulyiaFlenent analysisintu the resolve phase.MuVuAPuCJHuNuS.Heshun eat mine/% 2.23 13.0655.6229.0929.41 2.09 0.49 4.95Tbble 2 Rcsult of the Chemical Analysis of the Coal AshwwwwwwwwwwSiO2 Al2O, Fe(2 Cu0 Mg0 YHshun 时minei 53.27 31.46 4.22 4.74 1.13 94.82'The added amount of the sulfur-lixation agenl depended on the molar matio (2:1) of the Ha or Ca in thesulfur-fixation agent toS in the coul. The molar ratio ofsulfur-fixation agcnt to the assistant sulfur-fixation agent is100: 1. 'Ihe sample was kept in a resisance stove al850C , 950C, 1050C, 1I50C, 1250 and 1350C for30 minules after being skived and mised cormpletely , aundthe sulfur-fixation products were obtained. The S content▲CuSO。 ●Ca5i0。 ¥CaO. AL0, ■2CS. CaSO,of those producls were measured by the SC-132, aund thesulfur-fixation fficiency of sulfur-fixation agent was ob-Hig. 1 XRD ptters of the slfur frxation poduxt by CGa00tained. In order to study the crystallized behavior of thea:950CCa00 b:950CCGCQCO + Mg0,desulfurization of BaC0;, the combustion sulfur fixationc:950CGaCO, + si0O, d:15090a0, ,product of the rpresentatve sanple was analyzed aurd ob-e: J150(aC0 +S:00served by X-ray diraction (XRD) and scanning electronmieroscopy (SEM).3 Results and Discussion3. | X-ray analysis of sulfur fixation productwwhXRD patterms o[ the sulfur-fixation prvduct bhy Ca-C03 and BaC03 are shown in Fig. 1 and 2, in which wecan see that the adition of the asistant agent has n0 ap)-parcnt effect on the minerd-crystal components. CuSO,crystal minerals exist in the desulfurization product of theCaC03 at 9509; (Fig. la, b,e). Diffraction peaks of BaO. Al2O3 ,Al2O, . Si0, and BaS0, exist in the suluf-fixation▲3Ca0:3A20.R0Q2●Dt&S0,★Rd).A203■Ah2() Si0product of BaCO3 at 950C (Fig.2a,b,c). With the in-Hig.2 XRI) pttcons of the sfurfixalion produrt by BRaC0),crease of lcmperature. the dffaction peaks of CaSO. exista:980CBxC0, b:959CBbco + Mg0,in the slurfixation product of CaCO3 (Fig. ld,e) atc:950'CBaA + SrCO, d1150C.BaCO,e:1150CBu0O, + SrUX f:1400C RaXDh1150C, and simulaneously crystals of Ca.Si0. (a -CS),CS. CaSO4 and Ca0. Al203 cone into being. Dif-3.2 Analysis of microstructure of the sulfur fixationfraction peaks of Ba0 Al2O, and Al2O, . Si02 are replaceddregs'The representative sulfur-ixation products of BaCO,by those of the BaAl2 5i04 in the sulfur fixation product ofBaCO, , at the same time, dfraction peaks of the BaSO21150C and 1350C were selccted to be testod by SEM,inagcs of the rmicruslructure are shown in Figs. 3,4 andand 3CaO* 3Al203 " BaSO4 are found( big. 2d,e) . Increas-5ing the temperature to 1400C( Fig.20) , dffrction peaks中国煤化工soc, dhe nineralof BaS0, and 3Ca0- 3Al2O3●BaSO, still cxist in the sulfurerystal:fYHC N M H Gur-lixalion produc:t-. fixation dreg of BaCO,, but the itetesities of the dif-of CaC03There is grainy CxS in big.3(a,b),and C2Sfraction peaks decrease, which shows hat BaSO4 andincreases partially after Mg0 is added (Fig.3 b) , and pil-3Ca0- 3Al20. BaSO, have better stability at higher tcm-lar CaO- Al2O3 crytal prtally separate out after SrC03 is5eJourmnal of Wuhan Universily of Tehnology - Mater. Sei. Ed.Dee. 2003(a) CaCO,(b) CaCO,+Mg0的CaCO,+SrC0, .Fig.3 SEM images of the sulufixatin prochun:t by CaCO, in 1150C(a) BaC0,b) BaCO2+MgO的BaCO,+ScC0,Fig.4 SEM inegrs of the sfi-fixation prnduct by BaCO3 in 1150C201U万S.000 Fon 8810 J5M-56 1eLu203 X5.00 5 000J01H-561aC0206000(回) BaCO,6) BaCO,+MgO的BaCO.+SsCO,Fig.5 SEM inuges of the sulur-fixation produc1 by RaC0; in 1350Cadded (Fig.3 c).There is a bigger hole ratio in the sul-in the sulfur-fixation product of BaCO3,crystal phase in-fur- fixation product of BaCO, at 1150C( Fig 4) , and thecreases after Mg0 is added, while the rsolve phase de-crysladls scpanted oul are connected with each other . Reg- creases; the shape of polyhedral erystal with added SrC03ular brim can be seen at the section, and the integral ap-. ,mne without SrC0, , butpearance is similar with that o[ sulphale cement.The hole中国煤化工rapparently .ratio inerases after MgO is added (Fig.4 b) ; and crystalYHC N M H Gufur fixation processgrows after SrCO, is added (Fig.4 c). At 1350C(Fig.of sulfur-fixation agent5),polyhcdral crystals are wrapped by the resolve objextIt can be known from the above X-ray diffractionVol.18 No.4XIE Jun-lin el al :FRert of Additive on Sulur - fixation Process of...57analysis that when CaCOz and BaCO3 are used as the sul-crystal lttite defects in the solid, which include point de-fur-fixation agent, the additive assistant dcsulfurizationfects, planc defects and crystal disloxation, and the greatagent has no apparent ffet on the minucral-crystal compo-effet of the sive o[ the additive objecls or ions on the ionnents. F'rom the SEM images it can be seen that the addit-diffuse. When the elfect is bigger and the ion size isives change the separate ability of the crystal in the sulfur-smaller, the acceleration efet is apparent'。.Thc Mg* infixation pruduct of CaCO2. MgO acelerates the reaction o[MgO is smaller than Sr * in SrC0, so the activation ofSiO2 in the ash with CaO, and Sr0 acceleratcs the reactionMg0 to BaCO3 is super han that to SrC02.of AL2O, in the ash with CaO. In the sulfur fixation prod-4 Conclusionsuct of BaCO,,the additive changes the hole structure andthe liquid forming temperature, and results in an increasea) When CaCO, and BaCO3 wem: used as he sufur-o[ the content of mineral crystalline with a good slability.It can be concluded that the increase o[ sfur-fixation ca-fixation agenl , the adition of the assislant desulfurizationgenls had no apparent effecl on the mineral-crystal (01--pability for the addilive is not due to their direr reactionto form sllate or inlcraction with CaC0, and BaCO3 toponents.b) The added agent changed the separate ability ofform compusite minerl heat-resistant in high (emperature ,the crystals in the sufur-ixation prorduct by CaC0, .bul due to their activation lo sulfur fixation reaction of thec) The added agent increased the hole natrio and thesulfur- fixation agent.Prasannan et als. used the particles model to ex-liquiding lemperatur: of the sulfur-fixation product bhyplain how the presence of inpurity improves the lransla-BaCO3,and increased the amount separated outl o[ thetion ratio o[ solid reaction in n0u- ceatnlyzed raction. Themincrals crystals with a better stability.d) 'The improvcment of the uditive to the sufur fix-particles swell gradually with the reaction process . Whenthe reaction proceeds 10 a certain degree, prodluc:t fomedation fficiency was due l0 the activation of the aditve toby the pure purticles is much close,which is not beneficialthe sulfur-fixation raction.to the continuous difuse o{ the gas. While the productformed by the particles with inpurity is loos and thereReferencesare bigger holes , the decrnasing degree of the diffusc coef-Paolo Davini et al. Inluence of Sodium Chloride on the Desud-ficient is slower than that o[ the pure particles with thephriation Properties of limestone. F'uel,1992,71(3):831procoss of the raction , which contributes lo the reaction of! Gina K, Paul E. Sinmultancous Hot Dsulfizutioi and Imprvwedthe diffusion and the liquid phascs . Similar conclusionsFiltralion in (Cinal Uilication Proceses . Enivnmeruul Progress ,are drawn with tbe experimertls from another respect.1997, 16(2):93SrC03 and MgO existing on the Ba anrd Ca surfaces3 Wung Chunpuo el al . Desuphuriation Fxperiment und Anafysisand rvacting with CaO and Ba0 resolved from CaC03 andof GaO. HuaRei Unicersity of Kletrie Pouer Xrbu, 999, 26<2):85BaCO, , arceleral: the speed of the transfer and the diffuseLi Ning."The Eee of Clay Ore upon Desulphurialion of CaC0,of the metal ions , which results in the changes of the crys-at ligh Tempeature. Anivorment Pection, 198,(4);:43tal strueture of CaO and RaO. The lrules of Ca0 and Ba05 Prusannan PC. A Model for (iaus Solid Reactions with Sinucturebexume bigger, and more, which contributes to the difuseChargers in the Presernce of Inert Sovlid. Chem. eing. Sei., .of SO2,improving the sintering of (aO and BaO in high1985.40:1251temperalure region, recducing the jam chancs by CaSO,,6 Bongwardt R H, Bruce K R. An Investigation of Pruduel-layerHaSO, , and the sulfur-lixation product, and ten improvingifuivily for (a() ulaion. Ind. &Eng. Chem. 1987. 26( 10);1993the sulfur-fixation eficiency of the: sulfur-fixation agent.Ihe difusing rate of he ions is dependent on the .中国煤化工MYHCNMHG

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