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1.
载铁煤焦中铁化学形态的研究 总被引:3,自引:0,他引:3
利用EXAFS,XANES和XRD方法对负载三氯伦铁的地焦中铁化学形态进行了表征,并着重考察煤的铁负载量对铁化学形态的影响。在600℃热解条件下,两种褐煤载铁半焦中铁主要以晶相Fe3O4存在,而烟煤载铁半焦中以Fe3O4,FeO和α-Fe混合物相存在。 相似文献
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铁催化剂对煤热解过程中氮元素迁移的影响 总被引:11,自引:0,他引:11
应用XRD和EXAFS技术表征了热解温度对煤中铁催化剂形态的影响,用XPS表面分析方法研究了铁催化剂对煤热解过程中氮元素迁移的影响。结果表明:铁元素在低温制备煤焦中的主要物相是Fe2O3和Fe3O4,而在高温制备的煤焦中,还原态α-Fe和铁碳物种(Fe,C)是铁元素的主要存在形态。煤或焦中的氮元素以季胺盐、吡啶和吡咯等三种形态存在。铁能催化季胺盐在较低温度下分解。与吡咯类氮相比较而言,铁能优先催化 相似文献
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ELECTRON-TRANSFER IN POLYNUCLEAR CYANO-BRIDGED COMPLEX OF THE TYPE[Co(Ⅲ)L_3-μ-Nc-Fe(Ⅱ)(CN)_5]~-(L=en
《中国化学快报》1994,(11)
ELECTRON-TRANSFERINPOLYNUCLEARCYANO-BRIDGEDCOMPLEXOFTHETYPE[Co(Ⅲ)L_3-μ-Nc-FeⅡ)(CN)_5]~-(L=en)ShuZhongZHAN;XiaoYuanCHEN;QingJin?.. 相似文献
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聚丙烯腈脱氮碳化过程中负载铁的化学形态 总被引:2,自引:0,他引:2
应用EXAPF和XRD技术研究了负载聚丙烯腈有脱氮碳化过程中铁化学形态的变化,发现在300-1000℃范围内随碳化温度的升高,铁化学形态呈如一顺序递变;Fe3O4-Fe2.5N-Fe3C-α-Fe。 相似文献
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标题化合物(Me2SiSiMe2)〔η^5-(3-Me3SiC5H3)Fe(CO)2〕2/(μ-CO)2(A)分子中的Fe-Fe键被钠汞齐还原断裂,生成相应的双铁负离子,分别与MeCOCl、PhCOCl、PhCH2Cl、ClCH2COOC2H5和Ph3SnCl进行亲核取代反应,生成在铁原子上引入相应取代基的产物(Me2SiSiMe2)〔η^5-(3-Me3SiC5H3)Fe(CO)2R〕2(R:M 相似文献
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CRYSTAL STRUCTURE OF A 2D SHEET-LIKE μ-CYANIDO-OXAMIDATO BRIDGED Fe(III)-Cu(II) HETERNUCLEAR COMPLEX
《中国化学快报》1994,(8)
CRYSTALSTRUCTUREOFA2DSHEET-LIKEμ-CYANIDO-OXAMIDATOBRIDGEDFe(III)-Cu(II)HETERNUCLEARCOMPLEX¥NeiFangWu;ZhongNingCHEN;JunQIUandW... 相似文献
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先锋褐煤焦的铁催化CO2脉冲气化 总被引:1,自引:0,他引:1
利用脉冲反应技术研究了先锋褐煤焦CO2气化反应的铁催化作用,并考察了铁负载量,催化剂前体和制备方法对化活性的影响。研究结果表明,催化剂前体为Fe(NO3)3时活性最高FeC6H5O7次之,FeCl3最小。离子交换制备方法可显著提高FeCl3催化活性,这些因素主要表现在对煤焦表现催化剂浓度的影响,铁对碳化聚丙烯腈的C 气化具有异常高的催化活性,其活的种可能为铁碳化合物。 相似文献
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煤催化气化条件下不同煤种煤灰烧结行为研究 总被引:1,自引:0,他引:1
选取9类典型煤种,利用压差法测定烧结温度的实验装置,结合灰渣的XRD分析结果,考察了添加K基碱金属催化剂、不同煤种灰成分对烧结温度的影响。结果表明,碳酸钾催化剂的添加,明显降低高铁钙含量的WJT煤的灰熔点及烧结温度,碱金属K化合物极易同煤中Fe、Ca的矿物质反应生成低温共融物进而加剧煤灰的熔融结渣。不同煤种烧结温度的差异与煤灰中硅、铝、铁、钙含量密切相关。铝、硅含量高的煤灰烧结温度较高,而铁、钙含量高的煤灰烧结温度相对较低。碱金属K催化剂的添加加剧了煤灰的烧结结渣,而钙、铁的存在会加速硅铝酸盐间的反应生成低温共融物进而加速灰熔融。各煤种烧结温度的变化与其灰成分在CaO-SiO2-Al2O3、FeO-SiO2-Al2O3三元相图上的位置相吻合。 相似文献
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Mei Wu Huahua Zhao Jian Yang Jun Zhao Huanling Song Lingjun Chou 《Russian Journal of Physical Chemistry A, Focus on Chemistry》2017,91(11):2103-2109
The effect of iron precursor on the property and catalytic behavior of iron modified titanium silicalite molecular sieve (Fe-TS-1) catalysts in butadiene selective epoxidation has been studied. Three Fe-TS-1 catalysts were prepared, using iron nitrate, iron chloride and iron sulfate as precursors, which played an important role in adjusting the textural properties and chemical states of TS-1. Of the prepared Fe-TS-1 catalysts, those modified by iron nitrate (FN-TS-1) exhibited a significant enhanced performance in butadiene selective epoxidation compared to those derived from iron sulfate (FS-TS-1) or iron chloride (FC-TS-1) precursors. To obtain a deep understanding of their structure-performance relationship, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Temperature programmed desorption of NH3 (NH3-TPD), Diffuse reflectance UV–Vis spectra (DR UV–Vis), Fourier transformed infrared spectra (FT-IR) and thermal gravimetric analysis (TGA) were conducted to characterize Fe-TS-1 catalysts. Experimental results indicated that textural structures and acid sites of modified catalysts as well as the type of Fe species influenced by the precursors were all responsible for the activity and product distribution. 相似文献
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《Spectrochimica Acta Part B: Atomic Spectroscopy》2002,57(4):711-725
Both sulfur and iron chemical environments were studied in natural compounds; sulfides, sulfates and silicate basaltic glasses which are supposed to have variable oxidation states, using XANES (X-ray absorption near edge structure) spectroscopy. Although X-ray absorption methods are well suited for such investigations, the size of natural glass inclusions trapped in volcanic minerals, ranging from a few micrometers to several tenths of micrometers, makes micro-spectroscopy necessary. Hence, we present the μ-XANES spectra at the sulfur and iron K-edges of olivine-hosted glass inclusions containing from 1000 to 1650 ppm S, and between 5.5 and 7.8 wt.% Fe. By combining both high energy and spatial resolutions, we demonstrate the ability of the μ-XANES to produce quantitative determination of sulfur and iron valence states. We have identified various species for sulfur, specifically SII−, SVI and possibly SIV, in basaltic glass inclusions hosted in olivine grains. We propose a method to calibrate the proportion of Fe dissolved as Fe3+ in basaltic glasses for which the Fe3+/ΣFe ratio varies between 0.05 and 0.48 with a relative precision of less than 10%. 相似文献
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含铁骨架Fe-Al-EU-1分子筛的设计合成和晶化 总被引:2,自引:0,他引:2
以溴化六甲双铵(HMBr2)为模板剂,在HMBr2-Na2O-Al2O3-SiO2-Fe2O3-H2O体系中,采用水热法合成了高结晶度Fe-Al-EU-1分子筛,通过X射线粉末衍射(XRD)、扫描电子显微镜(SEM)、热重-微分热重(TG-DTG)分析、N2吸附-脱附、固体核磁共振(NMR)、紫外-可见(UV-Vis)吸收光谱和X射线吸收谱的精细结构(XAFS)等测试手段对合成样品的物理化学性质、铁在分子筛骨架的成键状态进行表征.结果表明:随着原始溶胶中铁的质量分数增加,Fe-Al-EU-1分子筛的晶胞体积增大;铁掺杂使Al-EU-1分子筛的表面积(BET)从272m2·g-1增加到365m2·g-1;模板剂脱除和分解温度降低;铁离子加入溶胶,导致zeta电位降低,胶体粒子容易聚集,分子筛外形增大.UV-Vis结果显示:由于220-250nm处的分子筛骨架中氧原子的成键2p电子向骨架四配位铁原子的空d轨道产生p-d跃迁,导致其特征峰的吸收峰强度急剧增加,在373nm左右骨架位的四配位铁原子与相邻的硅氧基团配位键合,产生能级分裂的d-d电荷跃迁峰且峰强度增加.XAFS结果表明:随着晶化过程的进行,边前1s→3d吸收峰和1s→4p主吸收峰发生了明显变化,原始溶胶样品在形成四配位铁物种结构单元后,逐步转化形成四面体配位的铁-硅-氧骨架铁物种,铁-硅-氧离子键结构单元也随之转变为四面体配位共价键结构的骨架铁物种. 相似文献
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Pyrazole, a neutral nitrogen ligand and an isomer of imidazole, has been used as a fifth ligand to prepare two new species, [Fe(TPP)(Hdmpz)] and [Fe(Tp-OCH(3)PP)(Hdmpz)] (Hdmpz = 3,5-dimethylpyrazole), the first structurally characterized examples of five-coordinate iron(II) porphyrinates with a nonimidazole neutral ligand. Both complexes are characterized by X-ray crystallography, and structures show common features for five-coordinate iron(II) species, such as an expanded porphyrinato core, large equatorial Fe-N(p) bond distances, and a significant out-of-plane displacement of the iron(II) atom. The Fe-N(pyrazole) and Fe-N(p) bond distances are similar to those in imidazole-ligated species. These suggest that the coordination abilities to iron(II) for imidazole and pyrazole are very similar even though pyrazole is less basic than imidazole. Mo?ssbauer studies reveal that [Fe(TPP)(Hdmpz)] has the same behavior as those of imidazole-ligated species, such as negative quadrupole splitting values and relative large asymmetry parameters. Both the structures and the Mo?ssbauer spectra suggest pyrazole-ligated five-coordinate iron(II) porphyrinates have the same electronic configuration as imidazole-ligated species. 相似文献
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Parra S Henao L Mielczarski E Mielczarski J Albers P Suvorova E Guindet J Kiwi J 《Langmuir : the ACS journal of surfaces and colloids》2004,20(13):5621-5629
A new type of Nafion/Fe structured membrane ensuring faster kinetics, higher efficiency, and mechanical properties has been prepared and will be compared in its performance with the Fe-exchanged commercial Dupont 117 Nafion/Fe membrane during the abatement of model organic compounds. During the casting of the laboratory Nafion sample, the iron ions were introduced directly into the Nafion oligomer solution. This novel laboratory Nafion/Fe was tested as an immobilized catalyst in the degradation of several toxic pollutants showing a faster photoassisted degradation kinetics and a wider effective photocatalytic pH range compared to the Fe-exchanged commercial Dupont 117 Nafion/Fe membrane. When carrying out Ar ion sputtering of the 50 topmost catalyst layers, evidence is presented by X-ray photoelectron spectroscopy that Fe ions are found in the inner Nafion layers and seem to be responsible for the immobilized photoassisted Fenton processes leading to the degradation of 4-chorophenol (4-CP) taken as a model organic pollutant for the degradation process reported in this study. In the laboratory sample, the iron oxy/hydroxy Nafion moiety undergoes a transition to a more stable Nafion/Fe species during 4-CP degradation as determined by X-ray diffraction. This more stable form shows a higher iron dispersion and crystallinity compared to the fresh sample and is stabilized by the Nafion matrix avoiding the formation of separate iron phases. By infrared absorption (Fourier transform infrared), evidence is presented for the band of akaganeite-like species at 870 cm(-1) on the laboratory Nafion/Fe sample. This band disappears after 4-CP degradation because of the formation of the more highly dispersed iron species. Sputtering experiments show a decrease of F-containing groups in the laboratory Nafion/Fe samples closer to the catalyst upper layer while the amounts of Fe, C, and in particular O species increase in the topmost layer(s). In particular, the oxygenated species develop in the Nafion/Fe up to approximately 50 A below the catalyst surface. These species remain stable during the long-term Nafion/Fe degradation of 4-CP. Dynamo-mechanical analysis performed on laboratory Nafion/ Fe membrane samples revealed that these membranes possessed a greater mechanical modulus and resistance than the commercial Dupont 117 Nafion membrane. 相似文献
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Cu-Co-Fe catalysts were prepared by coprecipitation of Cu-Co nitrate solutions with Na2CO3 and impregnation of iron nitrate on the Cu-Co precipitates by incipient wetness method; and their phase structure, composition and iron dispersion behavior were studied by XRD, SEM and SAM techniques. The catalyst precursor consists of CuO, Co3O4 and (-Fe2O3. The intensity of XRD peak of Fe2O3 changes as the relative content of iron varies. No X-ray diffraction peak of iron oxide appears unless the content of iron surpasses a threshold value. 相似文献
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采用液体离子交换、等体积浸渍和固相离子交换制备了一系列Fe-ZSM-5催化剂,并将其用于NH3选择性催化还原NOx(NH3-SCR)反应.运用X射线衍射、紫外-可见漫反射吸收光谱和原位漫反射傅里叶变换红外光谱对催化剂进行了表征.结果表明,Fe-ZSM-5催化剂表面Fe物种可分为孤立Fe3+物种、低聚Fe氧化物团簇和Fe2O3,各催化剂上NH3-SCR反应活性不同的根本原因是其表面Fe物种分布不同.水热老化后,Fe-ZSM-5催化剂上400oC以下反应时NOx转化率降低,而高温活性略有提高,各催化剂活性差异减小;同时NH3氧化活性和NO氧化活性均明显降低.这可归因于水热老化使Fe-ZSM-5催化剂表面的孤立Fe3+物种相对浓度降低,低聚Fe氧化物团簇和Fe2O3相对浓度增加,以及催化剂表面Br?nsted酸性位显著减少所致. 相似文献
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Linbo Xia Yingliang Wu Zucheng Jiang Shengqing Li Bin Hu 《International journal of environmental analytical chemistry》2013,93(11):953-962
The use of 1-phenyl-3-methyl-4-benzoylpyrazolone (PMBP) as extractant for separation of Fe(III) and Fe(II) and low-temperature vaporization of the Fe(III)–PMBP chelate into ICP-AES for their speciation analysis was investigated. The factors affecting the formation of Fe(PMBP)3 chelate and its vaporization behavior were investigated in detail. PMBP was used not only as the extractant for the separation of Fe(III) and Fe(II) but also as the chemical modifier for the low-temperature ETV-ICP-AES determination of iron. Under the optimized conditions, the detection limit for iron(III) and iron(II) are both 3.2?ng/mL, with relative standard deviations of 3.9 and 4.5%, respectively. The proposed method was applied to the determination of trace iron in biological standard reference materials and the species in East Lake water samples, and the results obtained were satisfactory. 相似文献