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1.
Regeneration of a high-temperature coal gas desulfurization sorbent is a key technology in its industrial applications. A Fe2O3-based high-temperature coal gas desulfurizer was prepared using red mud from steel factory. The influences of regeneration temperature, space velocity and regeneration gas concentration in SO2 atmosphere on regeneration performances of the desulfurization sorbent were tested in a fixed bed reactor. The changes of phase and the composition of the Fe2O3-based high-temperature coal gas desulfurization sorbent before and after regeneration were examined by X-ray diffraction (XRD) and X-ray Photoelectron spectroscopy(XPS), and the changes of pore structure were characterized by the mercury intrusion method. The results show that the major products are Fe3O4 and elemental sulfur; the influences of regeneration temperature, space velocity and SO2 concentration in inlet on regeneration performances and the changes of pore structure of the desulfurization sorbent before and after regeneration are visible. The desulfurization sorbent cannot be regenerated at 500°C in SO2 atmosphere. Within the range of 600°C–800°C, the time of regeneration becomes shorter, and the regeneration conversion increases as the temperature rises. The time of regeneration also becomes shorter, and the elemental sulfur content of tail gas increases as the SO2 concentration in inlet is increased. The increase in space velocity enhances the reactive course; the best VSP is 6000 h?1 for regeneration conversion. At 800°C, 20 vol-% SO2 and 6000 h?1, the regeneration conversion can reach nearly to 90%.  相似文献   

2.
Regeneration of a high-temperature coal gas desulfurization sorbent is a key technology in its industrial applications. A Fe2O3-based high-temperature coal gas desulfurizer was prepared using red mud from steel factory. The influences of regeneration temperature, space velocity and regeneration gas concentration in SO2 atmosphere on regeneration performances of the desulfurization sorbent were tested in a fixed bed reactor. The changes of phase and the composition of the Fe2O3-based high-temperature coal gas desulfurization sorbent before and after regeneration were examined by X-ray diffraction (XRD) and X-ray Photoelectron spectroscopy(XPS), and the changes of pore structure were characterized by the mercury intrusion method. The results show that the major products are Fe3O4 and elemental sulfur; the influences of regeneration temperature, space velocity and SO2 concentration in inlet on regeneration performances and the changes of pore structure of the desulfurization sorbent before and after regeneration are visible. The desulfurization sorbent cannot be regenerated at 500°C in SO2 atmosphere. Within the range of 600°C–800°C, the time of regeneration becomes shorter, and the regeneration conversion increases as the temperature rises. The time of regeneration also becomes shorter, and the elemental sulfur content of tail gas increases as the SO2 concentration in inlet is increased. The increase in space velocity enhances the reactive course; the best VSP is 6000 h−1 for regeneration conversion. At 800°C, 20 vol-% SO2 and 6000 h−1, the regeneration conversion can reach nearly to 90%.  相似文献   

3.
In this work, the H3PW12O40 heteropolyacid (HPW) was employed as a homogeneous catalyst to promote the efficient esterification (ethanolysis) of a number of saturated and unsaturated fatty acids (myristic, palmitic, stearic, oleic, and linoleic) under mild reaction conditions. HPW showed a similar activity to those observed for p-toluene sulfonic acid (PTSA) and sulfuric acid (H2SO4), the other acidic catalysts we compared them with in this study. In the HPW-catalyzed esterification of stearic acid, the addition of water caused a remarkable decrease in the ethyl stearate yields. On the other hand, the increase in the HPW concentration (up to a maximum value) promoted a proportional improvement in the oleic acid to ethyl oleate conversion. Kinetic measurements using oleic acid as a prototype substrate revealed that the esterification reactions catalyzed by HPW, H2SO4, and PTSA are of first-order in relation to the fatty acid concentration. Finally, the catalytic activity of HPW remained unaltered even after several recovery/reutilization cycles whereas the tungsten content in the final product (biodiesel produced by the HPW-catalyzed esterification of oleic acid) was found to be at an acceptably low level (0.0095 mg of W per g of biodiesel).  相似文献   

4.
H2 regeneration of an activated carbon supported vanadium and cobalt oxides (V2O5-CoO/AC) catalyst–sorbent used for flue gas SO2 removal is studied in this paper. Elemental sulfur is produced during the H2-regeneration when effluent gas of the regeneration is recycled back to the reactor. The regeneration conditions affect the regeneration efficiency and the elemental sulfur yield. The regeneration efficiency is the highest at 330 °C, with SO2 as the product. The production of elemental sulfur occurs at 350 °C and higher with the highest elemental sulfur yield of 9.8 mg-S/g-Cat. at 380 °C. A lower effluent gas recycle rate is beneficial to elemental sulfur production. Intermittent H2 feeding strategy can be used to control H2S concentration in the gas phase and increase the elemental sulfur yield. Two types of reactions occur in the regeneration, reduction of sulfuric acid to SO2 by AC and reduction of SO2 to elemental sulfur through Claus reaction. H2S is an intermediate, which is important for elemental sulfur formation and for conversion of CoO to CoS that catalyzes the Claus reaction. The catalyst–sorbent exhibits good stability in SO2 removal capacity and in elemental sulfur yield.  相似文献   

5.
The sulfur removing capacities of various Zn-Ti-based sorbents were investigated in the presence of H2O and HCl at high-(sulfidation, 650 °C; regeneration, 800 °C) and medium-(sulfidation, 480 °C; regeneration, 580 °C) temperature conditions. The H2O effect of all sorbents was not observed at high-temperature conditions. At mediumtemperature conditions, the reaction rate of ZT (Zn/Ti : 1.5) sorbent decreased with the level of H2O concentration, while modified (ZTC, ZTN) sorbents were not affected by the water vapor. HCl vapor resulted in the deactivation of ZT sorbent with a cycle number at high-temperature due to the production of ZnCl2 while the sulfur removing capacities of ZTC and ZTN sorbents were maintained during 4–5 cyclic tests. In the case of medium-temperature conditions, ZT sorbent was poisoned by HCl vapor while cobalt and nickel added to ZT sorbent played an important catalytic role to prevent from being poisoned by HCl due to providing heat, emitted when these additives quickly react with H2S even at medium-temperature conditions, to the sorbents  相似文献   

6.
SO_2对钙基吸收剂吸收NO的作用机理   总被引:1,自引:0,他引:1       下载免费PDF全文
针对低温条件下SO2对Ca(OH)2吸收NO的影响进行了实验研究,分析了烟气中O2和H2O对SO2促进Ca(OH)2吸收NO的影响。实验结果表明,当烟气不含SO2时,Ca(OH)2对NO基本无吸收作用;烟气中SO2的存在对NO吸收具有促进作用。H2O和O2对SO2促进NO吸收有显著影响;当烟气不含O2时,即使大量的SO2被吸收,NO吸收效率仍较低;只有SO2与O2和H2O共存才能促进NO吸收。脱硫产物CaSO3对NO无氧化作用;NO、H2O和SO2未在吸收剂表面产生可分解释放NO2的大分子中间配合物。分析认为在脱硫过程中产生了可以促进NO与O2反应的非稳定中间活性组分。  相似文献   

7.
Shengji Wu  Shinsuke Nagamine 《Fuel》2004,83(6):671-677
CaS formed from the CaO sorbent during desulfurization in coal gasifiers has to be converted to CaSO4 before disposal. CaS is mainly decomposed to CaO and SO2 by O2 and then CaO is converted to CaSO4 by SO2 and O2. The role of H2O in the oxidative decomposition of CaS with O2 was studied using reagent grade CaS and H218O. The following results were obtained: (1) there is a synergistic effect of H2O and O2 on the oxidative decomposition of CaS to CaO and SO2; (2) H2O reacts with CaS to form CaO, SO2 and H2 in the absence of O2; (3) the oxidative decomposition of CaS to CaO and SO2 occurs stepwise; (4) H2O directly reacts with CaS in the presence of O2; (5) H2O plays an important role in the oxidative decomposition of CaS even if the O2 concentration is high.  相似文献   

8.
The effect of the pretreatment (inert, oxidative, and reducing) of Ru/γ-Al2O3 catalyst on its activity and stability in the decomposition of N2O in the absence or presence of O2, SO2, H2O and NOX was studied in the present work. Decomposition of pure N2O was slightly enhanced by the H2-pretreated catalyst (metallic Ru) compared to the O2- or He-pretreated ones, owing to a cyclic oxidation–reduction pathway of metallic Ru. The observed decrease of activity by O2 or H2O addition was reversible compared to SO2 which caused a strong, irreversible deactivation of the catalyst, irrespective of the type of pretreatment. This was attributed to the formation of stable sulphates, mainly those on RuO2 surface, which could only be removed by regeneration under reducing (H2 in He) atmosphere at temperatures of ca. 500 °C. Oxidative or inert regeneration required very high temperatures (i.e. >700 °C) in order to decompose these sulphates. A method of retaining N2O conversion activity very high (≥98%) for long reaction times is suggested and is based on frequent and short-time (ca. 10 min) regenerations of the catalyst under reducing atmosphere (ca. 5% H2 in He). The effect of co-feeding various reducing agents, such as CO or C3H6, on the N2O conversion activity in the presence of O2, SO2, H2O and NOX is negligible, mainly because they are oxidized at relatively low temperatures in the O2-rich feeds used in this study.  相似文献   

9.
Removal of SO2 by activated carbon fibers in the presence of O2 and H2O   总被引:1,自引:0,他引:1  
Vivekanand Gaur 《Carbon》2006,44(1):46-60
This work describes the potential capability of activated carbon fibers (ACFs) in continuously removing SO2 from inert atmosphere without requiring further regeneration. A tubular reactor packed with ACF was used to study the conversion of SO2 into H2SO4 in the presence of O2 and H2O with varying concentrations of SO2 (3000-10,000 ppm), O2 (10-20%), and H2O (10-70%) and temperatures (313-348 K). The experiments were carried out on two precursors (viscose rayon and phenolic resin) based ACFs. The breakthrough data revealed that the steady-state SO2 concentration levels at the reactor exit increased with increasing inlet SO2 concentration and decreased with increasing concentration levels of O2 as well as H2O. Increase in the reaction temperature was found to moderately enhance the steady-state exit concentration levels of SO2. The viscose rayon-based ACF exhibited higher SO2 removal activity in comparison to the phenolic resin-based ACF. A mathematical model was developed to predict the gas concentration profiles in the reactor, incorporating the mass transfer in the bed as well as within the ACF pores, along with the surface reactions on the ACF. The model predictions agreed reasonably well with the data.  相似文献   

10.
To improve the poor SO2 absorption rate of CeFeMgTi sorbent with high sulfur removal capacity and fast regeneration, a new sorbent, CeFeMgTi-sol was prepared by the modified co-precipitation method and tested in a packed bed reactor at RFCC conditions (sulfation of MgO to MgSO4 in the presence of low concentration of SO2 at 973 K, regeneration of MgSO4 to MgO and H2S in the presence of H2 at 803 K). The CeFeMgTi-sol sorbent showed excellent SO2 absorption and sulfur removal capacity (46.2 sulfur g/g absorbent×100). It was found that the SO2 absorption rates were related to the structure of the Mg and Ti and the textural properties such as surface area and pore volume. In the case of the fresh state of CeFeMgTi sorbent, CeO2, MgO and MgTiO3 structures were observed. But the new CeFeMgTisol sorbent before SO2 absorption, showed a separated MgO and TiO2 peak only. These differences in the sorption rates were discussed by the difference in the XRD pattern, surface area and pore volume.  相似文献   

11.
Supporting V2O5 onto an activated coke (AC) has been reported to significantly increase the AC's activity in simultaneous SO2 and NO removal from flue gas. To understand the role of V2O5 on SO2 removal, V2O5/AC is studied through SO2 removal reaction, surface analysis, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared (FTIR) techniques. It is found that the main role of V2O5 in SO2 removal over V2O5/AC is to catalyze SO2 oxidation through a VOSO4-like intermediate species, which reacts with O2 to form SO3 and V2O5. The SO3 formed transfers from the V sites to AC sites and then reacts with H2O to form H2SO4. At low V2O5 loadings, a V atom is able to catalyze as many as 8 SO2 molecules to SO3. At high V2O5 loadings, however, the number of SO2 molecules catalyzed by a V atom is much less, due possibly to excessive amounts of V2O5 sites in comparison to the pores available for SO3 and H2SO4 storage.  相似文献   

12.
Hierarchical porous NiO/Al2O3 composites were successfully prepared by two-steps. First, the core-shell structured Al2O3 microspheres were prepared via a template-free hydrothermal route using KAl(SO4)2·12H2O and Al2(SO4)3·18H2O as aluminum source. Then, the NiO/Al2O3 composites with micro- and nano-hierarchical structures were prepared by a hydrothermal method combining the subsequent calcination process. The obtained characterization result presented that the morphology of hierarchical Al2O3 microsphere tuned to irregular platelets by simply varying Ni/Al ratios. The BET analysis showed that the special surface area from 52.12m2 g?1 to 214.8m2 g?1 after two hydrothermal complex process. Effects of Ni/Al ratio, adsorbent dosage, Congo red (CR) concentration, coexisting ions, adsorption time and temperature were investigated. The obtained results indicated that NiO/Al2O3 composite had the high adsorption efficiency (99.6%) and great adsorption capacity (186.9mg g?1) under the optimum conditions. The adsorption isotherm and kinetics data were found to be well fitted and in good agreement with the Langmuir isotherm model and pseudo-second order model, respectively. The hierarchical porous NiO/Al2O3 composites presented remarkably higher adsorption efficiency during five recycling, which showed their potential as the highly efficient adsorbent for removal of CR in wastewater.  相似文献   

13.
Xinyan Xing  Zhenyu Liu  Jianli Yang 《Fuel》2008,87(8-9):1705-1710
Flue gas SO2 removal at 200 °C over Mo and Co doped V2O5/AC catalyst-sorbents and regeneration of the used catalyst-sorbents in H2 at 380 °C in the same reactor are studied in this paper. Compared with V2O5/AC, the catalyst-sorbents containing Co show higher SO2 uptake while the one containing Mo shows a slightly lower SO2 uptake. Elemental sulfur is produced during H2-regeneration of the used catalyst-sorbents when effluent gas of the regeneration is recycled back to the reactor. H2-regeneration of the used V2O5/AC produces little elemental sulfur, but the Mo and Co doped ones show high elemental sulfur yields with an elemental sulfur selectivity of 50% for a catalyst-sorbent containing 2% V2O5, 0.5% MoO3 and 0.5% CoO, V2Mo0.5 Co0.5/AC. Molybdenum and cobalt sulfides are likely formed in the regeneration, which catalyze the elemental sulfur formation but reduce the SO2 uptake of the catalyst-sorbents in the subsequent SO2 removal stage.  相似文献   

14.
H2O2 vapor sterilization is an effective and safe method for removing various pathogens. To improve the efficiency of this technique, the time required for sterilization must be shortened. The aeration time constitutes a large portion of the total sterilization time; therefore, the development of a catalyst for H2O2 decomposition is necessary. Bulk MnO2 is typically used in H2O2 decomposition, but it has a low specific surface area. To increase H2O2 decomposition activity, specific surface area and electron transfer ability of catalyst need improvement. In this study, MnO2/CNT(x), where x denotes the weight ratio of CTAB to H2O in the catalyst preparation, was synthesized using a soft template method with varying amounts of the template. Overall, the catalyst specific surface area remarkably increased to 190–200 m2/g from 0.043 m2/g for bulk MnO2 and these increased surface areas resulted in superior H2O2 decomposition activity. Among the CNT-supported catalysts tested, MnO2/CNT (1.0) exhibited the highest activity, which was 570 times that of bulk MnO2. Aeration times were also calculated with some assumptions and the aeration can be finished within 1 hr (bulk MnO2 needs about 25 hr).  相似文献   

15.
An improved desulfurization process for removing sulfur from hydro treated diesel oil based on the oxidation of thiophenic type sulfur-containing compounds with H2O2 and acetic acid (AcOH) using H2SO4 as catalyst has been studied. The experimental results show that the sulfone content in the oxidation product increased rapidly with an increase in acetic acid and sulfuric acid ratios from 1:0 to 2:1 mole ratios. The maximum DBT conversion (wt.%) was at 2:1 mole ratio of acetic acid/sulfuric acid. This oxidation process is found to be capable of removing up to 90% of the sulfur compounds in hydro treated real fuels and can provide an alternative way to meet the future sulfur environmental requirements.  相似文献   

16.
The concentration dependence of the electrical conductivity of glasses in the Tl2O-B2O3 system is studied. The nature of charge carriers in this system is experimentally investigated for the first time. It is demonstrated using the Hittorf, Tubandt, and Hebb-Liang-Wagner techniques and the Faraday law that neither Tl+ ions nor electrons are involved in the electricity transport. The verification of the Faraday law does not reveal the presence of thallium in the amalgam of the cathode or a change in the sample weight after electrolysis, to within the experimental error. This allows one to make the inference that protons can be charge carriers in glasses of the Tl2O-B2O3 system. It is shown using extended X-ray absorption fine structure (EXAFS) spectroscopy that Tl3+ ions and thallium Tl0 reduced to the metallic state are absent in the structure of the glasses under investigation. This means that thallium in glasses of the Tl2O-B2O3 system occurs only in the form of Tl+ ions. The analysis of the IR spectroscopic data leads to only a qualitative conclusion that the water content in the glasses insignificantly increases with an increase in the thallium oxide content. An increase in the electrical conductivity of glasses in the Tl2O-B2O3 system with an increase in the thallium oxide content is explained by the increase in the number of protons formed upon dissociation of H+[BO4/2]? structural-chemical units, because their concentration increases with increasing Tl2O content. In the structure of boron oxide, impurity hydrogen enters predominantly into the composition of H+[O2/2BO?] structural-chemical units, for which the dissociation energy is higher than that for the H+[BO4/2]? structural-chemical units. The increase in the concentration of H+[BO4/2]? structural-chemical units is accompanied by the increase in the number of dissociated protons, which are charge carriers in glasses of the Tl2O-B2O3 system.  相似文献   

17.
The 0D-1D Lithium titanate (Li4Ti5O12) heterogeneous nanostructures were synthesized through the solvothermal reaction using lithium hydroxide monohydrate (Li(OH)·H2O) and protonated trititanate (H2Ti3O7) nanowires as the templates in an ethanol/water mixed solvent with subsequent heat treatment. A scanning electron microscope (SEM) and a high resolution transmission electron microscope (HRTEM) were used to reveal that the Li4Ti5O12 powders had 0D-1D heterogeneous nanostructures with nanoparticles (0D) on the surface of wires (1D). The composition of the mixed solvents and the volume ratio of ethanol modulated the primary particle size of the Li4Ti5O12 nanoparticles. The Li4Ti5O12 heterogeneous nanostructures exhibited good capacity retention of 125 mAh/g after 500 cycles at 1C and a superior high-rate performance of 114 mAh/g at 20C.  相似文献   

18.
Methods for regenerating H3PW12O40 catalyst in the solvent-free direct preparation of dichloropropanol (DCP) from glycerol and hydrochloric acid gas were investigated. Regenerated H3PW12O40 catalyst was then applied to the solvent-free direct preparation of DCP. In the solvent-free direct preparation of DCP, selectivity for DCP over H3PW12O40 catalyst regenerated by method I (recovery of solid H3PW12O40 catalyst by evaporating homogeneous liquidphase product solution) significantly decreased with increasing recycling run, while that over H3PW12O40 catalyst regenerated by method II (regeneration of H3PW12O40 catalyst by oxidative calcination of solid product recovered by method I) was slightly decreased with no significant catalyst deactivation with respect to recycling run. On the other hand, selectivity for DCP over H3PW12O40 catalyst regenerated by method III (regeneration of H3PW12O40 catalyst by recrystallization and subsequent oxidative calcination of solid product recovered by method II) was the same as that over fresh catalyst without any catalyst deactivation with respect to recycling run. Thus, method III was found to be the most efficient method for the regeneration of H3PW12O40 catalyst.  相似文献   

19.
The formation of N2O has been studied by means of isothermal lean-rich experiments at 150, 180 and 250 °C over Pt–Ba/Al2O3 and Pt/Al2O3 catalysts with H2 and/or C3H6 as reductants. This allows to provide further insights on the mechanistic aspects of N2O formation and on the influence of the storage component. Both gas phase analysis and surface species studies by operando FT-IR spectroscopy were performed. N2O evolution is observed at both lean-to-rich (primary N2O) and rich-to-lean (secondary N2O) transitions. The production of both primary and secondary N2O decreases by increasing the temperature. The presence of Ba markedly decreases secondary N2O formation. FT-IR analysis shows the presence of adsorbed ammonia at the end of the rich phase only for Pt/Al2O3 catalyst. These results suggest that: (i) primary N2O is formed when undissociated NO in the gas phase and partially reduced metal sites are present; (ii) secondary N2O originates from reaction between adsorbed NH3 and residual NOx at the beginning of the lean phase. Moreover, N2O reduction was studied performing temperature programming temperature experiments with H2, NH3 and C3H6 as reducing agents. The reduction is completely selective to nitrogen and occurs at temperature higher than 250 °C in the case of Pt–Ba/Al2O3 catalyst, while lower temperatures are detected for Pt/Al2O3 catalyst. The reactivity order of the reductants is the same for the two catalysts, being hydrogen the more efficient and propylene the less one. Having H2 a high reactivity in the reduction of N2O, it could react with N2O when the regeneration front is developing. Moreover, also ammonia present downstream to the H2 front could react with N2O, even if the reaction with stored NOx seems more efficient.  相似文献   

20.
TiO2 nanotubes promoted with Pt metal were prepared and tested to be the photocatalytic dehydrogenation catalyst in neat ethanol for producing H2 gas (C2H5OHC3CHO +H2). It was found that the ability to produce H2, the liquid phase product distribution and the catlyst stability of these promoted nano catalysts all depended on the Pt loading and catalyst preparation procedure. These Pt/TiO2 catalysts with TiO2 nanotubes washed with diluted H2SO4 solution produced 1, 2-diethoxy ethane (acetal) as the major liquid phase product, while over those washed with diluted HCl solution or H2O, acetaldehyde was the major liquid phase product.  相似文献   

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