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用穆斯堡尔谱初步探索煤液化时铁系催化剂的作用
A PRELIMINARY MSSBAUER SPECTROSCOPIC STUDY OF THE CATALYTIC ACTION OF IRON BASED CATALYSTS IN LIGNITE LIQUEFACTION
【摘要】 本文利用穆斯堡尔谱探索了黄铁矿和磁铁矿-硫在褐煤液化反应中的催化作用,得出在液化条件下,黄铁矿完全转变成FeS1+x,磁铁矿-硫或经过中间状态FeS2或直接转化成FeS1+x,两者在液化过程中都产生活性的H2S和FeS1+x,可催化煤炭液化反应。
【Abstract】 Catalytic actions of Qingsan pyrite and Chengchao fine ore(magnetite)on Xiaolongtan lignite liquefaction were studied with M(?)ssbauer spectro-meter.Lignite liquefaction was carried out in a microautoclave.Threeg coal,0.6g iron ore,0.06g sulfur(all minus 200 mesh)and 8ml solvents(tetralin:decalin=1:3(vol.))were put into the microautoclave whichhad been purged by N2 after assembling and pressurized to 5.9 MPaby H2.The microautoclave was then put into a sandbath and preheatedto 420℃.After 30 min of heating,the content of the microautoclavewas moved out and extracted with tetrahydrofuran(THF)in a Soxhletextractor for 24 h.The THF insoluble residue was dried in a 110℃oven for 2 h and then pulverized to minus 200 mesh.The residue wasprepared to a sample containing 10mgFe/cm2 which was analysed byM(?)ssbauer spectrometer under room temperature.The M(?)ssbauer spectro-meter used in this work was a conventional constant-acceleration instru-ment,the γ-source consisted of 50 mCi of 57Co in a Pd matrix.The zerovelocity is given with respect to a-Fe.Mssbauer spectra were analysedusing an STM computer assuming Lorentzian profile.The M(?)ssbauerparameters used in this work are the isomer shift(IS),the quadrupolesplitting(QS),and the magnetic hyperfine splitting.It has been observed that under conditions of the liquefaction,pyritewas decomposed into pyrrhotite,and magnetite-sulphur was transformedinto pyrrhotite directly or through the intermediate state of FeS2.Catalyticactions of the two minerals were similar,all producing active H2S andFeS1+x in the liquefaction process.For pyrite FeS2+(1-x)H2(gas)→FeS1+x+(1-x)H2SFor magnetiteFe3O4+(4+2x)S(melt)+4H2(gas)→FeS2+2FeS1+xFeS2+(1-x)H2(gas)→FeS1+x+(1-x)H2SThe catalytic actions were discussed,it is conjectured that active H2Sand FeS1+x contribute to the increased conversion of coal liquefactionwith iron-based catalyst.
- 【文献出处】 燃料化学学报 ,Journal of Fuel Chemistry and Technology , 编辑部邮箱 ,1988年01期
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