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File： s10163-022-01564-w.pdf

DOI： 10.1007/s10163-022-01564-w

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File： s40831-021-00489-2.pdf

DOI： 10.1007/s40831-021-00489-2

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Language：Japanese   Publishing type：Research paper (conference, symposium, etc.)  

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DOI： 10.1016/j.inoche.2020.108400

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DOI： 10.1016/j.polymdegradstab.2020.109225

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DOI： 10.1021/acs.iecr.9b00594

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DOI： 10.1021/acs.energyfuels.8b00838

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DOI： 10.1016/j.fuel.2018.01.069Get

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DOI： 10.3775/jie.97.31

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DOI： 10.1016/j.jece.2017.12.065

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DOI： 10.2355/isijinternational.ISIJINT-2017-190

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DOI： 10.1016/j.ultsonch.2017.08.023

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DOI： 10.2355/tetsutohagane.TETSU-2015-100

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Language：English   Publisher：IRON STEEL INST JAPAN KEIDANREN KAIKAN  

In order to understand the effect of down flow in RH ladle on mixing time, the relationship among flow patterns, circulation and mixing phenomena were examined by using three sizes of model RH. The temporal change in electric conductivity in ion-exchanged water was tracked after injecting KCI solution and the decoloration process of iodine color in ion-exchanged water was observed visually after injecting sodium thiosulfate solution. There were two mixing patterns in the ladle: One has a damping oscillation curve for a tracer response and the decoloration reaction occurred everywhere and uniformly, the other has a monotonical decreasing tracer curve after an overshoot and the decoloration delayed near the free surface of the ladle. The (t(m)/t(R))/(D-leg/H) values decreased with the increase in Re below Re1.8x 104 and it was kept to be constant above Re-i- -1.8x 10(4) where tm: a mixing time (s), tR: a mean residence time (s) of fluid in the ladle, Dieg: inner diameter of down -leg (m) and H: length of jet axis between down -leg outlet and jet-impinged wall (m). In the region of Re > 1.8x10(4), the mixing was controlled by the circulating flow, whereas in the region of Re <1.8x10(4) the mixing behavior was influenced by the stagnation zone near the free surface of the ladle.

DOI： 10.2355/isijinternational.ISIJINT-2015-714

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Language：English   Publisher：ELSEVIER SCIENCE BV  

Activated carbon (AC) is an organic adsorbent and mostly used to adsorb volatile organic compound pollutants. In the present work, AC was produced from rubber wood sawdust via a physical activation method using CO2 gas. Prior to activation process, the biomass was carbonized under N-2 gas flow of 600 mL/min for 1 h at a corresponding temperature to produce char. The effect of activation temperature (700, 720, 740, and 760 degrees C) and time (60, 90, and 120 min) on the mass yield and characteristics of activated carbon was investigated. In overall, the yield of AC decreased when heated at higher activation temperature and increased at longer time. Under nitrogen adsorption analysis, surface area and pore volume of AC were determined. At higher temperature, surface area and pore volume increased, but excessive heating could break the pore structure. Next, the performance of activated carbon was tested in term of adsorption capacity for gas and liquid phase adsorption represented by benzene and trichloroethylene, respectively. Preliminary results suggested that the AC could adsorb both compounds efficiently. (C) 2016 The Authors. Published by Elsevier Ltd.

DOI： 10.1016/j.proeng.2016.06.549

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Language：English   Publisher：AMER CHEMICAL SOC  

The effect of the presence of HCl and SO2 in the simulated coal combustion flue gas on the Hg-0 removal by a commercial activated carbon (coconut shell AC) was investigated in a laboratory-scale fixed-bed reactor in a temperature range of 80-200 degrees C. The characteristics (thermal stability) of the mercury species formed on the sorbents under various adsorption conditions were investigated by the temperature-programmed decomposition desorption (TPDD) technique. It was found that the presence of HCl and SO2 in the flue gas affected the mercury removal efficiency of the sorbents as well as the characteristics of the mercury adsorption species. The mercury removal rate of AC increased with the HCl concentration in the flue gas. In the presence of HCl and the absence of SO2 during Hg-0 adsorption by AC, a single Hg-0 desorption peak at around 300 degrees C was observed in the TPDD spectra and intensity of this peak increased with the HCl concentration during mercury adsorption. The peak at around 300 degrees C may be derived from the decomposition and desorption of mercury chloride species. The presence of SO2 during mercury adsorption had an adverse effect on the mercury removal by AC in the presence of HCl. In the presence of both HCl and SO2 during Hg-0 adsorption by AC, the major TPDD peak temperatures changed drastically depending upon the concentration of HCl and SO2 in flue gas during Hg-0 adsorption.

DOI： 10.1021/ef900057e

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Language：English   Publisher：ELSEVIER SCIENCE BV  

Low temperature selective catalytic reduction (LT-SCR) of NO+NO2 mixture with NH3 was investigated over TiO2, SiO2 and activated carbon in a conventional flow type fixed-bed reactor at 100 degrees C under atmospheric pressure. The effects of gas composition such as presence of SO2 and NH3 and the ratio of NO2/NO in the feed-stream on the LT-SCR have been studied. The presence of SO2 and O-2 was essential for the selective removal of NO with NH3 over TiO2. The presence of SO2 contributed to the oxidation of NO to NO2 over TiO2. If NO2 existed with NO in the reaction system, the presence of SO2 was not necessary for the removal of NO over TiO2. The following two reactions were suggested to occur over TiO2: NO+NO2 + 2NH(3) -> 2N(2) + 3H(2)O (1) and 2NO(2) +2NH(3) -> N-2 + NH4NO3 + H2O (2). The reaction (2) occurred on all three catalysts, however the reaction (1) did not proceed significantly over SiO2. (C) 2009 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.molcata.2009.06.002

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Language：English   Publisher：AMER CHEMICAL SOC  

Catalytic gasification of wood biomass was carried out using a double-bed microreactor in a two-stage process. Temperature-programmed steam gasification of biomass was performed in the first bed at 200-850 degrees C. Following in series was isothermal catalytic decomposition and gasification of volatile compounds (including tars) in the second bed containing various dolomites. Dolomites from Canada, Australia, and Japan were examined for their effects on tar conversion and the overall gaseous product. A total of 74% of biomass carbon was emitted as volatile matter during tar gasification (200-500 degrees C biomass bed temperature). Dolomites improved tar conversion to gaseous products by an average of 21 % over noncatalytic results at a 750 degrees C isothermal catalyst bed temperature using 1.6 cm(3) dolomite/g of biomass. The iron content in dolomite was found to promote tar conversion and the water-gas shift reaction, but the effectiveness reached a plateau at 0.9 wt % Fe in Canadian dolomites. The maximum tar conversion of 66% was achieved at 750 degrees C using a Canadian dolomite with 0.9 wt % Fe (1.6 cm(3)/g of biomass). Carbon conversion to gaseous products increased to 97% using 3.2 cm(3) dolomite/g of biomass at the same temperature. The dolomite seemed stable after 15 h of cyclic use at 800 degrees C.

DOI： 10.1021/ef8009958

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Language：English   Publisher：ELSEVIER SCI LTD  

Development of an elemental mercury (Hg-0) removal process for coal derived fuel gas is an important issue in the development of a clean and highly efficient coal power generation system. Recently, iron-based sorbents such as iron oxide (Fe2O3), Supported iron oxide on TiO2, and iron disulfide have been proposed as active mercury sorbents. It was supposed that Hg-0 reacted with H2S on the iron-based sorbents and captured mercury. However, the mercury species captured on the sorbents have not been directly characterized yet. The captured mercury species was too small to identify because the concentration of Hg-0 was very low (ppb order). In this study, a temperature programmed decomposition technique is applied in order to understand the decomposition character of the mercury species captured on iron-based sorbents. The Hg-0 removal experiments were carried out in a laboratory-scale fixed-bed reactor at 80 degrees C using simulated fuel gas. After the Hg-0 removal experiments, desorption of the captured mercury species was carried out in the same fixed-bed reactor using an atomic absorption spectrophotometer. Temperature programmed decomposition desorption (TPDD) experiments revealed that the decomposition characteristic of mercury species captured on the sorbent was similar to that of HgS reagents (cinnabar and meta-cinnabar). Furthermore, it was observed that the characteristics of the decomposition of mercury species depended on the sorbent type of sorbents and reaction conditions. (C) 2008 Elsevier Ltd. All rights reserved.

DOI： 10.1016/j.fuel.2008.06.011

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High calcium content peat was used for the preparation of activated carbons with CO2 activation. The influence of temperature on the porous characteristics of the activated carbons was investigated. Calcium compounds were found to intensify the pore widening at high temperatures. As a result, the micropore volumes and surface areas of the samples prepared at 850 degrees C were lower than those prepared at 650 and 750 degrees C. As the mesopores were destroyed at high temperature, the total pore volume decreased at 850 degrees C and was lower than at 750 degrees C. (C) 2008 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.jaap.2008.07.001

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Language：English   Publisher：AMER CHEMICAL SOC  

In order to clarify the role Of SO2 in the removal of mercury from coal combustion flue gas by activated carbon, the removal of Hg-0 vapor from simulated coal combustion flue gas containing SO2 by a commercial activated carbon (AC) was studied. ne Hgo removal experiments were carried out in a conventional flow type packed bed reactor system with simulated flue gases having a composition of Hg-0 (4.9 ppb), SO2 (0 or 500 ppm), CO2 (10%), H2O (0 or 15%), O-2 (0 or 5%), and N-2 (balance gas) at a space velocity (SV) of 6.0 X 10(4) h(-1) in a temperature rang 60- 100 degrees C. It was found that, for SO2 containing flue gas, the presence of both O-2 and H2O was necessary for the removal of Hgo and the Hgo removal was favored by lowering the reaction temperature in the order of 60 > 80 > 100 degrees C. The presence of SO2 in the flue was essential for the removal of HgO by untreated activated carbon. The activated carbons pretreated with SO2 or H2SO4 Prior to the HgO removal also showed Hgo removal activities even in the absence of SO2; however, the presence of SO2 also suppressed the Hgo removal of the SO2-pretreated AC or H2SO4 preadded AC.

DOI： 10.1021/ef800134t

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Language：English   Publisher：ELSEVIER SCI LTD  

Catalytic gasification of wood (Cedar) biomass was carried out using a specially designed flow-type double beds micro reactor in a two step process: temperature programmed non-catalytic steam gasification of biomass was performed in the first (top) bed at 200-850 degrees C followed by catalytic decomposition gasification of volatile matters (including tars) in the second (bottom) bed at a constant temperature, mainly 600 degrees C. Iron oxide catalysts, which transformed to Fe3O4 after use possessed catalytic activity in biomass tar decomposition. Above 90% of the volatile matters was gasified by the use of iron oxide catalyst (prepared from FeCl3 and NH3aq) at SV of 4.5 x 10(3) h(-1). Tar was decomposed over the iron oxide catalysts followed by water gas shift reaction. Surface area of the iron oxide seemed to be an important factor for the catalytic tar decomposition. The activity of the iron oxide catalysts for tar decomposition seemed stable with cyclic use but the activity of the catalysts for the water gas shift reaction decreased with repeated use. (c) 2007 Elsevier Ltd. All rights reserved.

DOI： 10.1016/j.fuel.2007.06.021

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Laboratory studies were conducted to develop an elemental mercury (Hg-0) removal process based on the reaction of H2S and Hg-0 using iron-based sorbents for coal derived fuel gas. It is well known that hydrogen chloride (HCl) is present in fuel gases derived from some types of coal, but the effect of HCI on the Hg-0 removal performance of iron-based sorbents in coal derived fuel gas is not yet well understood. In this study, the effects of HCl on the removal of Hg-0 from coal derived fuel gases over iron-based sorbents such as iron oxide (Fe2O3) supported iron oxides on TiO2, iron oxide-Ca(OH)(2), and iron sulfides were investigated. The Hg-0 removal experiments were carried out in a laboratory-scale fixed-bed reactor at 80 degrees C using simulated fuel gas. In the case of iron oxide (Fe(2)o(3)), the presence of HCl suppressed the Hg-0 removal rate. In the case of Fe2O3 (2 or 5 wt%)/TiO2, the presence of HCl did not suppress the Hg-0 removal rate and the activity was stable. The Hg-0 removal performance of reagent FeS2 was higher than that of the iron oxide, and not affected by the presence of HCI. The Hg-0 removal rate of iron oxide-Ca(OH)(2) was not effected by the presence of HCI, because HCl was captured by Ca(OH)(2). The reagent FeS2 showed higher Hg-0 removal activity than that of FeS2 ore. However, the Hgo removal performance of ground and kneaded FeS2 ore was comparable to that of reagent FeS2 probably due to the increase in porosity of the FeS2 ore by grinding and kneading. (c) 2007 Elsevier Ltd. All rights reserved.

DOI： 10.1016/j.fuel.2007.06.016

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The aim of this study is to develop a process for the removal of Hg-0 using H2S over iron oxides sorbents, which will be located just before the wet desulfurization unit and catalytic COS converter of a coal gasification system. It is necessary to understand the reactions between the iron oxide sorbent and other components of the fuel gas such as H2S, CO, H-2, H2O, etc- In this study, the sulfidation behavior and activity for COS formation during Hg-0 removal from coal derived fuel gas over iron oxides prepared by precipitation and supported iron oxide (I wt% Fe2O3/TiO2) prepared by conventional impregnation were investigated. The iron oxide samples were dried at 110 degrees C (designated as Fe(2)O3-110) and calcined at 300 and 550 degrees C (Fe2O3-300 and Fe2O3-550). The sulfidation behavior of iron oxide sorbents in coal derived fuel gas was investigated by thermo-gravimetric analysis (TGA). COS formation during Hg-0 removal over iron oxide sorbents was also investigated using a laboratory-scale fixed-bed reactor. It was seen that the Hg-0 removal activity of the sorbents increased with the decrease of calcinations temperature of iron oxide and extent of sulfidation of the sorbents also increased with the decrease of calcination temperature. The presence of CO suppressed the weight gain of iron oxide due to sulfidation. COS was formed during the Hg-0 removal experiments over Fe2O3-110. However, in the cases of calcined iron oxides (Fe2O3-300, Fe2O3-550) and I wt% Fe2O3/TiO2, formation of COS was not observed but the Hg-0 removal activity of 1 wt% Fe2O3/TiO2 was high. Both FeS and FeS2 were active for Hg-0 removal in coal derived fuel gas without forming any COS. (c) 2007 Elsevier Ltd. All rights reserved.

DOI： 10.1016/j.fuel.2007.03.004

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Activated carbons were prepared by the pyrolysis of a mixture of fly ash and road paving asphalt dissolved in kerosene at 650 degrees C in N-2 atmosphere. Asphalt provides a porous carbonaceous structure and also acts as a binder to hold the fly ash particles together. The fly ash acts as a support for this carbon structure. The preparation variables studied were the pretreatment of asphalt-fly ash composite in air or N-2; and the asphalt ratio (amount of asphalt in grams added to 100 g of fly ash) of the raw mixture. The pretreatment of asphalt-fly ash composite at 250 degrees C in air resulted in a higher effective asphalt carbon yield than no pretreatment or pretreatment in N-2. The effective asphalt carbon yield increased with asphalt ratio up to 20 and then decreased at higher ratios. For heavy oil fly ash, the optimum asphalt ratio was 50-60 for maximum carbon yield. The specific surface areas of the asphalt and fly ash carbons were in the range of 500-800 m(2)/(g-asphalt derived carbon), depending on the asphalt derived carbon content of the sample. The asphalt ratio in the raw materials also affected the macropore structure of the product carbon: the macropore diameter of the sample increased with asphalt ratio. (c) 2006 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.jaap.2006.09.004

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Language：English   Publisher：AMER CHEMICAL SOC  

TiO2 is known as a low-temperature selective catalyst for the reduction (LT-SCR) of NO with NH3. Furthermore, it is well-known that the oxidation of NO over the catalyst plays an important role in the LT-SCR. Adsorption of SO2 and NO over two kinds of TiO2 catalysts was investigated using a conventional flow type fixed-bed reactor at 100 degrees C under atmospheric pressure. The effect of the presence of SO2 on the adsorption of NO over the catalysts and the formation NO2 from NO was studied. The relationship between the NO2 formation, the NO adsorption, and the SO2 adsorption was also studied. The presence of SO2 was essential for the oxidative adsorption of NO over the catalysts. SO2 was adsorbed and converted to SO42-, then NO adsorbed on the SO2 pre-adsorbed catalyst and converted to NO3-. The presence of both SO2 and NO contributed to the formation NO2 from NO over the TiO2 samples. It was found that NO2 was evolved from an equimolar reaction of NO and SO2.

DOI： 10.1021/ie061631q

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The characteristics of a novel method for Hg removal using H2S and sorbents containing iron oxide were studied. Previously, we have suggested that this method is based on the reaction of Hg and H2S over the sorbents to form HgS. However, the reaction mechanism is not well understood. In this work, the characteristics of the Hg removal were studied to clarify the reaction mechanism. In laboratory made sorbents containing iron oxide were used as the sorbent to remove mercury vapor from simulated coal derived fuel gases having a composition of Hg (4.8 ppb), H2S (400 ppm), CO (30%), H-2 (20%), H2O (8%), and N-2 (balance gas). The following results were obtained: (1) The presence of H2S was indispensable for the removal of Hg from coal derived fuel gas; (2) Hg was removed effectively by the sorbents containing iron oxide in the temperature range of 60-100 degrees C; (3) The presence of H2O suppressed the Hg removal activity; (4) The presence of oxygen may play very important role in the Hg removal and; (5) Formation of elemental sulfur was observed upon heating of the used sample. (c) 2005 Published by Elsevier Ltd.

DOI： 10.1016/j.fuel.2005.01.020

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Removal of Hg-0 vapor from the simulated coal combustion flue gases with a commercial activated carbon was investigated using H2S. This method is based on the reaction of H2S and Hg over the adsorbents. The Hg-0 removal experiments were carried out in a conventional flow type packed bed reactor system in the temperature range of 80-150 degrees C using simulated flue gases having the composition of Hg-0 (4.9 ppb), H2S (0-20 ppm), SO2 (0-487 ppm), CO2 (10%), H2O (0-15%), O-2 (0-5%), N-2 (balance gas). The following results were obtained: in the presence of both H2S and SO2, Hg removal was favored at lower temperatures (80-100 degrees C). At 150 degrees C, presence of O-2 was indispensable for Hg-0 removal from H2S-SO2 flue gas system. It is suggested that the partial oxidation of H2S with O-2 to elemental sulfur (H2S + 1/2O(2) = S-ad + H2O) and the Clause reaction (SO2 + 2H(2)S = 3S(ad) + 2H(2)O) may contribute to the Hg-0 removal over activated carbon by the following reaction: S-ad + Hg = HgS. The formation of elemental sulfur on the activated carbon was confirmed by a visual observation. (c) 2005 Elsevier Ltd. All rights reserved.

DOI： 10.1016/j.fuel.2005.04.007

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Hydrodehalogenation of CBrClF2, CCl2F2, CHClF2, and CH2F2 with hydrogen has been studied in the gas phase and over supported Pd catalysts in a tubular alumina reactor. During gas-phase reactions, selectivity to CH2F2 is low for the hydrodehalogenation of CBrClF2, CCl2F2, and CHClF2. CHClF2 is the primary product for the hydrodehalogenation of CBrClF2 and CCl2F2, whereas C2F4 is the major product for the hydrodehalogenation of CHClF2. Over Pd/C catalysts, CH2F2 is the primary product, with selectivities generally over 60% for the hydrodehalogenation of CBrClF2, CCl2F2, and CHClF2. Halocarbons and hydrogen compete for the available surface sites on Pd, and it is suggested that the rate-limiting step during the catalytic hydrodehalogenation of the four halocarbons involves the cleavage of C-halogen bonds, that is, C-Br in CBrClF2, C-Cl in CCl2F2 and CHClF2, and C-F in CH2F2.

DOI： 10.1021/ie049228b

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Language：English   Publisher：WILEY-BLACKWELL  

Thermal pyrolysis of halon 1211 (CBrClF2), diluted in nitrogen, in a tubular alumina reactor, has been studied over the temperature range of 773-1073 K at residence times from 03 to 2 s. At temperatures below 973 K, the major products were CCl2F2, CBr2F2, C2Cl2F4, C2BrClF4, C2F4, and C2Br2F4. Further increasing temperature resulted in the formation of CBrF3, CClF3, and many other species whose formation necessitated the rupture of C-F bonds. Coke formation was also observed on the surface of the reactor at high temperatures. A kinetic reaction scheme involving 16 species and 25 reaction steps was developed and applied to model the thermal pyrolysis of halon 12 11 over the temperature range of 773-973 K. Sensitivity analysis suggests that the reaction CBrClF2 + CClF2 --> CCl2F2 + CBrF2 constitutes the major pathway for the decomposition of halon 1211 under the conditions investigated. (C) 2005 Wiley Periodicals, Inc.

DOI： 10.1002/kin.20055

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The thermal and catalytic degradation of a complex polymer mixture was performed at 450degreesC at atmospheric pressure in a batch process. The mixture contained polyethylene (PE), polypropylene (PP), polystyrene (PS), acrylonitrile-butadiene-styrene copolymer with a brominated flame retardant and antimony oxide synergist (ABS-Br) and poly(vinyl chloride) (PVC), in a 3/3/ 2/1/1 weight ratio. The effect of iron (FeOOH and Fe-C composite) and calcium (CaCO3 and Ca-C composite) based catalysts for removal of heteroatom- (nitrogen, bromine, and chlorine) containing compounds in oil products was studied. Changes in the amount and distribution of heteroatoms were described using NP gram curves. Iron catalysts give best results for bromine removal from decomposition oil while calcium catalysts have high efficiency for chlorine removal; however, both Fe- and Ca-catalysts have low effect in nitrogen removal. Carbon composite catalysts give three times less chlorine but they produce higher amounts of nitrogen in degradation oils than the corresponding Fe and Ca pure compounds. In bromine removal Ca-C composite shows higher effect compared to CaCO3 while Fe-C composite has slightly worse effect than FeOOH. (C) 2004 Elsevier Ltd. All rights reserved.

DOI： 10.1016/j.polymdegradstab.2004.08.008

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Conversion of halon 1211 has been studied over gamma-Al2O3 and supported 0.5% Pd catalysts (Pd/Al2O3, Pd/fluorinated Al2O3, Pd/AlF3, Pd/ Al2O3 pretreated with CH4 and CHCIF2). The experiments were performed in the temperature range of 443-523 K, in a tubular alumina reactor. The temperature of the reactor was maintained uniformly by a three zone furnace. The reaction products were quantified with a micro gas chromatograph and identified with a gas chromatograph-mass spectrometer. The catalysts were characterised with XRD diffractometry and the content of halogen on the catalysts was determined with an ion chromatograph. The measurements were presented in terms of the conversion of halon 1211 and product selectivity, as functions of catalyst type, catalyst time on stream and composition of inlet gases. Transformation of Pd to Pd carbide is observed in the CH4 treated Pd/Al2O3, but not in the CHCIF2 treated Pd/Al2O3 in which case Al2O3 was partially fluorinated. In the absence of hydrogen, the conversion of halon 1211 over Al2O3 and Pd/Al2O3 gives a similar product profile and the reactions follow a heterogeneous halogen exchange reaction pathway, which takes place on the positively charged aluminum ions. Introduction of hydrogen has no apparent effect on either halon 1211 conversion level or the product profile during the conversion of halon 1211 over Al2O3. Over supported Pd catalysts, major products are hydrogenated species which include CH2F2, CH4, C2H6, C3H8, CH3Br and CHF3. The most striking feature of the hydrodehalogenation reactions is the increasing CH2F2 selectivity with time on stream, especially on Pd/Al2O3 and the CH4 treated Pd/Al2O3. The changing selectivity during the catalytic hydrodehalogenation reactions is mainly ascribed to the interaction of support with Pd. (C) 2004 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.cattod.2004.03.069

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Complex polymer mixtures of high density polyethylene (PE), polypropylene (PP), polystyrene (PS) and acrylonitrile-butadiene-styrene copolymer containing a polybrominated epoxy type flame retardant (ABS-Br) were thermally degraded at 450 degreesC in the presence of PVC and/or PET. It was found that besides a large amount of styrene and benzene derivatives (more than 50 wl.%), the pyrolysis oils contained about 1000 ppm nitrogen, 1000-4000 ppm bromine, 5000-5200 ppm chlorine and 800-1300 ppm oxygen, their amount and distribution depending on the composition of polymer mixture. The effect of PVC manifests especially in the early stages of decomposition while PET influenced also the late stages of the process. ABS copolymer and its flame retardant interact with both PVC and PET during thermal decomposition. (C) 2004 Elsevier Ltd. All rights reserved.

DOI： 10.1016/j.fuel.2004.04.011

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Language：English   Publisher：PERGAMON-ELSEVIER SCIENCE LTD  

Acrylonitrile-butadiene-styrene (ABS) copolymers without and with a polybrominated epoxy type flame retardant were thermally degraded at 450 degreesC alone (10 g) and mixed with polyvinylchloride (PVC) (8 g/2 g). Gaseous and liquid products of degradation were analysed by various gas chromatographic methods (GC with TCD, FID, AED, MSD) in order to determine the individual and cumulative effect of bromine and chlorine on the quality and quantity of degradation compounds. It was found that nitrogen, chlorine, bromine and oxygen are present as organic compounds in liquid products, their quantity depends on the pyrolysed polymer or polymer mixture. Bromophenol and dibromophenols were the main brominated compounds that come from the flame retardant. 1-Chloroethylbenzene was the main chlorine compound observed in liquid products. It was also determined that interactions appear at high temperatures during decomposition between the flame retardant, PVC and the ABS copolymer. (C) 2004 Elsevier Ltd. All rights reserved.

DOI： 10.1016/j.chemosphere.2004.04.002

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Pyrolysis of polypropylene (PP)/polyethylene (PE)/polystyrene (PS)/poly(vinyl chloride) (PVC)/high impact polystyrene with brominated flame retardant (HIPS-Br) plastics mixed with poly(ethylene terephthalate) (PET) was performed at 430degreesC under atmospheric pressure using a semi-batch operation. The presence of PET in the pyrolysis mixture of PP/PE/PS/PVC/HIPS-Br affected significantly the formation of decomposition products and the decomposition behavior of the plastic mixture. We observed the following effects of PET on the pyrolysis of PP/PE/PS/PVC/HIPS-Br mixed plastics: (i) the yield of liquid product decreased and the formation of gaseous products increased; (ii) a waxy residue was formed in addition to the solid carbon residue; (iii) the formation of SbBr3 was not detected in liquid products; (iv) the yield of chlorinated branched alkanes increased as well as vinyl bromide and ethyl bromide were formed. The use of calcium carbonate carbon composite (Ca-C) completely removed the chlorine and bromine content from the liquid products during PP/PE/PS/PVC/HIPS-Br pyrolysis, however in the presence of PET, the catalytic experiment (Ca-C, 8 g) yielded liquid products containing 310 ppm of Br and 20 ppm of Cl. In addition, the Ca-C increased the yield of liquid products about 3-6 wt.%, as well as enhanced the gaseous product evolution and decreased the yield of residue. The halogen free liquid hydrocarbons can be used as a feedstock in a refinery or as a fuel. (C) 2004 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.jaap.2004.01.005

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Polymer mixtures containing 8 g of high density polyethylene (PE) or polystyrene (PS) and 2 g of acrylonitrile-butadiene-styrene copolymer containing a polybrominated epoxy type flame retardant (ABS-Br) were thermally degraded at 450degreesC. FeOOH and two carbon composites based on iron (Fe-C) and calcium (Ca-C) were used for catalytic decomposition and their effect on the bromine and nitrogen amount and distribution in pyrolysis oil was determined by GC-AED analysis. It was found that iron-based catalysts removed bromine from pyrolysis oil and decreased the nitrogen amount converting nitrile compounds into ammonia. Calcium carbon composite had lower effect especially on the pyrolysis of PS/ABS-Br mixture. These liquid products can be used as fuel oil or feedstock in petroleum refinery. (C) 2004 Elsevier Ltd. All rights reserved.

DOI： 10.1016/j.polymdegradstab.2004.02.003

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The pyrolysis of brominated flame retardant containing high impact polystyrene (HIPS-Br) mixed with poly(ethylene terephthalate) (PET) was performed at 430degreesC under atmospheric pressure by a batch operation. The addition of PET to HIPS-Br affected significantly the formation of decomposition products and the degradation behavior of HIPS-Br. We have found the following observations on the addition of PET during the pyrolysis of HIPS-Br: (i) the rate of formation and the yield of liquid products decreased, (ii) the residue and gaseous products formation increased, (iii) the average carbon number (Cnp) of liquid products reduced from 12.5 to 9.1, (iv) the yield of high molecular weight hydrocarbons (C-16-C-20) decreased and the amount of hydrocarbons from C-6 to C-10 doubled, (v) heavy waxy compounds were formed on the top of the glass reactor wall in addition to the solid residue on the bottom of the reactor, (vi) antimony compounds were observed in the solid residue, as opposed to the formation of antimony tribromide (SbBr3) detected in the liquid products of HIPS-Br in the absence of PET. We attempted the debromination of brominated liquid hydrocarbons using iron and calcium based carbon composites for the production of halogen free liquid hydrocarbons, which can be used as a feedstock in a refinery or as a fuel. (C) 2003 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.jaap.2003.10.006

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Language：English   Publisher：ELSEVIER SCI LTD  

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 O-2 and then CaO is converted to CaSO4 by SO2 and O. The role of H2O in the oxidative decomposition of CaS with O-2 was studied using reagent grade CaS and (H2O)-O-18. The following results were obtained: (1) there is a synergistic effect of H2O and O-2 on the oxidative decomposition of CaS to CaO and SO2; (2) H2O reacts with CaS to form CaO, SO2 and H-2 in the absence of O-2; (3) the oxidative decomposition of CaS to CaO and SO2 Occurs stepwise; (4) H2O directly reacts with CaS in the presence of O-2; (5) H2O plays an important role in the oxidative decomposition of CaS even if the O-2 concentration is high. (C) 2003 Elsevier Ltd. All rights reserved.

DOI： 10.1016/j.fuel.2003.10.027

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Language：English   Publisher：ELSEVIER SCIENCE BV  

TiP2O7 carbon composite photocatalyst was successfully prepared by using ion-exchanged resin (C467) containing amino phosphate by metal ion-exchanged carbothermal reduction (MIER-CTR) method using TiCl3 and TiCl4. During the carbonization process in nitrogen, the pre-oxidation (300-350degreesC) in air is essential for producing homogeneously dispersed TiP2O7 on the carbon matrix. In the absence of pre-oxidation. the resin was melted. The carbonization temperature 500degreesC was found to be suitable for producing single phase TiP2O7 with higher yields. Powder X-ray diffraction (XRD) and Raman spectroscopic results suggest the formation of TiP2O7, while X-ray diffraction results reveal that the crystallite size was less than 35 nm. UV-Vis studies show that the band gap of TiP2O7 was 3.32 eV. The TiP2O7 carbon composite catalyst was applied for the photocatalytic decomposition of 2-propanol at 30degreesC using a mercury lamp (365 nm). (C) 2003 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.apcata.2003.10.047

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Language：English   Publisher：AMER CHEMICAL SOC  

Low-temperature hydrothermal treatment of waste biomass (sawdust) was performed using an autoclave at various temperatures of 180, 250, and 280 degreesC for 15 min and 60 min. The oil product was obtained from both liquid and solid portions of reaction products from the autoclave, and the composition of oil products was investigated separately. At high reaction temperature, i.e., 250 degreesC and 280 degreesC, the longer reaction time led to decreased oil yield; at low reaction temperature (180 degreesC), the oil yield was found to increase with the increase of reaction time. The oil1 (extracted from the liquid portion) consists of low-boiling-point compounds, whereas oil2 (extracted from the solid portion) contained both low- and high-boiling-point oxygenated hydrocarbons. Ca(OH)(2) was found to be effective on liquefaction of biomass in terms of both oil yield and composition. The volatility distribution of oxygenated hydrocarbons in oil1 and oil2 was studied by using a C-NP gram which can be used as a tool for characterizing biomass-derived oil products.

DOI： 10.1021/ef030133g

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Language：Japanese   Publisher：Japan Institute of Energy  

A unique technique to characterize the hydrocarbon fuel oil was developed and called "NPgram", for Normal Paraffin gram. This technique was applied to characterize coal derived oil mostly composed of aromatics. The NPgrams of S, N, Cl, and O-compounds in coal derived oils were shown. The NPgrams of these heterogeneous compounds were obtained by plotting the amount of heterogeneous compounds determined by GC-AED (Atomic Emission Detector) against the carbon number.

DOI： 10.3775/jie.83.56

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Language：English   Publisher：Elsevier Science Publishers B.V.  

The dechlorination of chloroorganic compounds from PVC-containing mixed plastic-derived oil was studied over iron oxide and iron oxide-carbon composite catalysts. The catalysts are characterized by nitrogen adsorption and X-ray diffraction. The catalysts are deactivated initially due to the adsorption of HCl gas that is produced during the reaction. Continuous adsorption of HCl on iron oxide leads to the conversion of iron oxide to iron chloride. The catalysts' deactivation was overcome by removing the reversible adsorbed HCl gas continuously, using He as a carrier gas.

DOI： 10.1016/S0926-860X(00)00656-6

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Language：English   Publisher：Elsevier Science Publishers B.V.  

The dechlorination of chloroorganic compounds from PVC-containing mixed plastic-derived oil was studied over iron oxide and iron oxide-carbon composite catalysts. The catalysts are characterized by nitrogen adsorption and X-ray diffraction. The catalysts are deactivated initially due to the adsorption of HCl gas that is produced during the reaction. Continuous adsorption of HCl on iron oxide leads to the conversion of iron oxide to iron chloride. The catalysts' deactivation was overcome by removing the reversible adsorbed HCl gas continuously, using He as a carrier gas.

DOI： 10.1016/S0926-860X(00)00656-6

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Language：English  

Ni-carbon composite catalysts were prepared by a modified carbothermal reduction method using ion exchange resins. The catalysts were characterised by N2 adsorption, X-ray diffraction and transmission electron microscope. The catalysts activities and selectivities were studied in the hydrodechlorination of chlorobenzene. The catalyst activities depend upon the carbothermal reduction temperature during preparation. These catalysts are found to be more stable and selective in this reaction even in the presence of HCl which is produced during the reaction. (C) 2000 Elsevier Science B.V.

DOI： 10.1016/S1381-1169(00)00328-9

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Language：English   Publisher：AMER CHEMICAL SOC  

The thermal degradation of the acrylonitrile-butadiene-styrene copolymer (ABS) was carried out at different temperatures from 360 to 440 degrees C in static and dynamic atmospheres of nitrogen, using semibatch operation. Nitrogen-containing compounds were found in all three degradation fractions: gases (as NH3 and HCN), oil, and residue. The percentage of the oil fraction increases with the increase of the degradation temperature. At 440 degrees C 63 wt % of the initial ABS feed was recovered in the oil fraction. The nitrogen (N) concentration of the oil fraction was in the range of 29-40 mg/mL. 4-Phenylbutyronitrile is the main N-containing degradation product (16-19 wt % in oil). N-compounds were also found as aliphatic and aromatic nitriles, amino derivatives, and heterocyclic compounds containing one or two N atoms such as pyridine, pyrimidine, and quinoline. Dynamic atmospheres of nitrogen and the residence time of the products in the reactor affects the oil recovery rate and the distribution of N in the degradation products.

DOI： 10.1021/ef000018v

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Language：English   Publisher：AMER CHEMICAL SOC  

The thermal degradation of the acrylonitrile-butadiene-styrene copolymer (ABS) was carried out at different temperatures from 360 to 440 degrees C in static and dynamic atmospheres of nitrogen, using semibatch operation. Nitrogen-containing compounds were found in all three degradation fractions: gases (as NH3 and HCN), oil, and residue. The percentage of the oil fraction increases with the increase of the degradation temperature. At 440 degrees C 63 wt % of the initial ABS feed was recovered in the oil fraction. The nitrogen (N) concentration of the oil fraction was in the range of 29-40 mg/mL. 4-Phenylbutyronitrile is the main N-containing degradation product (16-19 wt % in oil). N-compounds were also found as aliphatic and aromatic nitriles, amino derivatives, and heterocyclic compounds containing one or two N atoms such as pyridine, pyrimidine, and quinoline. Dynamic atmospheres of nitrogen and the residence time of the products in the reactor affects the oil recovery rate and the distribution of N in the degradation products.

DOI： 10.1021/ef000018v

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Language：English   Publisher：Chemical Society of Japan  

A selective vapour phase dehydrochlorination (DHC) of chloro alkanes was achieved over a simple iron oxide catalyst system. The chloro alkanes were selectively dehydrochlorinated to their corresponding alkenes. This catalyst was also found to be effective for the removal of chlorine from fuel oil derived from the degradation of PVC containing waste plastics.

DOI： 10.1246/cl.1999.1321

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Language：English   Publisher：Chemical Society of Japan  

A selective vapour phase dehydrochlorination (DHC) of chloro alkanes was achieved over a simple iron oxide catalyst system. The chloro alkanes were selectively dehydrochlorinated to their corresponding alkenes. This catalyst was also found to be effective for the removal of chlorine from fuel oil derived from the degradation of PVC containing waste plastics.

DOI： 10.1246/cl.1999.1321

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Language：English   Publisher：American Chemical Society  

This work deals with the investigation of the conditions under which a spontaneous degradation municipal waste plastic containing poly(vinyl chloride) (PVC) occurs during the dechlorination on an experimental scale by batch operation using a glass reactor, paying particular attention to the gas-solid reaction between the hydrogen chloride deriving from the PVC and the aluminum foil contained in the waste plastics. On the basis of observation of the effect of the rate of heating and the mode of contact between the PVC and aluminum foil on the change in the plastic melted level in the reactor, we were able to reproduce the spontaneous degradation of plastics with the production of a waxlike substance at around 593 K and at atmospheric pressure. The reason for the occurrence of spontaneous reaction was concluded to be the formation of "hot spots" (localized heating) originating from the heat of reaction between HCl generated from PVC and Al foil which eventually triggered the drastic thermal degradation of melted plastics. The possible conditions for the occurrence of the unusual reaction were discussed. © 1998 American Chemical Society.

DOI： 10.1021/ie9709392

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Language：English   Publisher：Elsevier Ltd  

The degradation of four different types of polyethylene (PE) namely high density PE (HDPE), low density PE (LDPE), linear low density PE (LLDPE), and cross-linked PE (XLPE) was carried out at 430°C by batch operation using silica-alumina as a solid acid catalyst and thermally without any catalyst. For thermal degradation, both HDPE and XLPE produced a significant amount of wax-like compounds and the yields of liquid products (58-63 wt%) were lower than that of LDPE and LLDPE (76-77 wt%). LDPE and LLDPE produced a very small amount of wax-like compounds. Thus the structure of the degrading polymers influenced the product yields. The liquid products from thermal degradation were broadly distributed in the carbon fraction of n-C5 to n-C25 (boiling point range, 36-405°C). With silica-alumina, all of the polyethylenes were converted to liquid products with high yields (77-83 wt%) and without any wax production. The liquid products were distributed in the range of n-C5 to n-C20 (mostly C5-C12). A solid acid catalyst indiscriminately degraded the various types of polyethylene into light fuel oil with an improved rate. © 1997 Elsevier Science Limited. All rights reserved.

DOI： 10.1016/S0141-3910(96)00191-7

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Language：English   Publisher：Elsevier  

The thermal degradation of plastic polymers into fuel oil over mesoporous silica (KFS-16) catalyst has been investigated. The product yields, composition and degradation rate of polyethylene over KFS-16 were compared with those over solid acid catalyst (silica-alumina and zeolite) and non-catalytic thermal degradation. The initial rate of degradation of PE over KFS-16, which possesses no acid sites was as fast as that over silica-alumina (SA-1) and the yield of liquid products was higher. The composition of the liquid products of degradation over KFS-16 was different from that over SA-1 and similar to that of non-catalytic thermal degradation. SA-1 catalyst deactivated very rapidly due to coke deposition, whereas KFS-16 deactivated much more slowly. These findings over mesoporous silica suggest that the mesopores surrounded by the silica sheet may act as a flask for storing radical species for a long time and then long-lived radicals accelerate the degradation of plastics. © 1997 Elsevier Science B.V.

DOI： 10.1016/S0165-2370(97)00052-1

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Language：English   Publisher：Elsevier Ltd  

Thermal degradation of plastics such as polyethylene (PE), poly(vinylchloride) (PVC), poly(ethyleneterephthalate) (PET) and their mixtures (PE + PVC and PE + PET) was studied at 430°C by batch operation to analyse the conversion of waste plastics into fuel oil. A visual inspection of the inside of the reactor was made and the macroscopic process of degradation was monitored. Products of degradation were classified into three groups: gases, liquids and residues in the reactor. The degradation of PE produced liquid products which consisted of C5-C25 fraction of hydrocarbons with a yield of 70 wt%. On the other hand, the degradation of PVC produced only 4.7 wt% liquid products which consisted of C5-C20 fraction of hydrocarbons and the degradation of PET produced no liquid products. The effect of mixing PVC and PET with PE on the yield and compositions of liquid products was investigated. The addition of either PVC or PET to PE decreased the overall liquid products yield
however, it promoted the degradation of PE into low molecular weight liquid hydrocarbon products. © 1996 Published by Elsevier Science Limited.

DOI： 10.1016/0141-3910(96)00077-8

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In order to understand the behavior of COS in the ZnS zone of a packed bed high-temperature desulfurization reactor, the catalytic character of ZnS for the conversion of COS to H2S in the presence of gases which are composed of coal-derived gas was studied. ZnS was active for the catalytic hydrolysis of COS in simulated coal-derived gases
ZnS was also active for the hydrogenation of COS to H2S, but the activity was considerably lower than that for the hydrolysis of COS. In simulated coal-derived gases, ZnS was also active for the reverse reaction
H2S was converted to COS over ZnS. The water gas shift reaction did not proceed in parallel with hydrolysis of COS over ZnS. From the results of this work, it is suggested that if the contact time of COS with ZnS was sufficient, the equilibrium of the conversion of COS to H2S was controlled by the following reaction: 2COS + H2 + H2O ↔ 2H2S + CO + CO2. © 1995, American Chemical Society. All rights reserved.

DOI： 10.1021/ie00043a011

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In order to understand the behavior of COS in the ZnS zone of a packed bed high-temperature desulfurization reactor, the catalytic character of ZnS for the conversion of COS to H2S in the presence of gases which are composed of coal-derived gas was studied. ZnS was active for the catalytic hydrolysis of COS in simulated coal-derived gases
ZnS was also active for the hydrogenation of COS to H2S, but the activity was considerably lower than that for the hydrolysis of COS. In simulated coal-derived gases, ZnS was also active for the reverse reaction
H2S was converted to COS over ZnS. The water gas shift reaction did not proceed in parallel with hydrolysis of COS over ZnS. From the results of this work, it is suggested that if the contact time of COS with ZnS was sufficient, the equilibrium of the conversion of COS to H2S was controlled by the following reaction: 2COS + H2 + H2O ↔ 2H2S + CO + CO2. © 1995, American Chemical Society. All rights reserved.

DOI： 10.1021/ie00043a011

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Language：English  

Soot formation over zinc ferrite high-temperature desulfurization sorbents was examined. When active zinc ferrites were used in simulated coal-derived gases for fuel cells, a large amount of soot was formed over the ferrites. This soot formation decreased with the increase of reaction temperature. This soot formation was inhibited by H2O and CO2 and accelerated by H2 and CO. These dependencies of the rate of soot formation on the concentration of H2O, CO2, H2, and CO can be expressed by six experimental equations. Carbides (Fe3C- and Fe3C-like compound, FexC) were found in the sample over which soot was formed. Fibrous ZnO was formed over the surface of the sample when the sample ZnFe2O4 was converted to carbides (Fe3C and FexC). It is thought that the carbides and the soot were produced via a surface active carbon. © 1995, American Chemical Society. All rights reserved.

DOI： 10.1021/ef00050a020

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The catalytic properties of framework Fe3+ in MFI-type H-ferrisilicate for the selective reduction of nitric oxide with ammonia in the presence of oxygen have been investigated and compared with those of Fe-exchanged ZSM-5, iron oxide supported on silicalite and HZSM-5. H-ferrisilicate exhibited a high activity and selectivity for the reduction of nitric oxide into nitrogen. A side reaction, i.e. the oxidation of ammonia with oxygen into nitrogen, occurred only above 773 K. The activity and selectivity of Fe-exchanged ZSM-5 for the reduction of nitric oxide were comparable to those of H-ferrisilicate, while iron oxide supported on silicalite catalysed the oxidation of ammonia with oxygen into nitric oxide preferentially under the same reaction conditions. The catalytic activity of HZSM-5 for this reaction was much lower than that of H-ferrisilicate. Therefore, the framework Fe3+ ions in H-ferrisilicate are the active sites for the selective catalytic reduction of nitric oxide.

DOI： 10.1039/FT9959103275

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Soot formation over zinc ferrite high-temperature desulfurization sorbents was examined. When active zinc ferrites were used in simulated coal-derived gases for fuel cells, a large amount of soot was formed over the ferrites. This soot formation decreased with the increase of reaction temperature. This soot formation was inhibited by H2O and CO2 and accelerated by H2 and CO. These dependencies of the rate of soot formation on the concentration of H2O, CO2, H2, and CO can be expressed by six experimental equations. Carbides (Fe3C- and Fe3C-like compound, FexC) were found in the sample over which soot was formed. Fibrous ZnO was formed over the surface of the sample when the sample ZnFe2O4 was converted to carbides (Fe3C and FexC). It is thought that the carbides and the soot were produced via a surface active carbon. © 1995, American Chemical Society. All rights reserved.

DOI： 10.1021/ef00050a020

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The catalytic activity of framework iron in MFI-type ferrisilicate was studied. The incorporation of Fe3+ ions in the tetrahedral framework of MFI-type ferrisilicate was investigated by means of Mössbauer spectroscopy. The derived Mössbauer parameter at room temperature clearly indicated the presence of Fe3+ ions in tetrahedral lattice sites. The catalytic activity of ferrisilicate was tested for the oxidation of CO with O2 at 673 K and was compared with the activities of iron-oxide-impregnated silicalite (FeOx/Sil) and Fe ion-exchanged ZSM-5 (FeZSM-5). The CO oxidation activity of the tetrahedrally coordinated Fe3+ in ferrisilicate was much lower than that of octahedrally coordinated Fe3+ in FeOx/Sil and Fe3+ in ion-exchange sites of FeZSM-5. Kinetic studies were performed on these catalysts at 623 K. On ferrisilicate, the reaction orders for CO and O2 were 1.0 and 1.1, respectively, while on FeOx and FeZSM-5 the reaction orders were 1.3 and 1.2 for CO, respectively, and near zero for O2 in both cases. For CO oxidation, both the activity and reaction mechanism on ferrisilicate differed markedly from those on FeOx/Sil and FeZSM-5. © 1993.

DOI： 10.1016/0927-6513(93)80078-9

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The catalytic activity of framework iron in MFI-type ferrisilicate was studied. The incorporation of Fe3+ ions in the tetrahedral framework of MFI-type ferrisilicate was investigated by means of Mössbauer spectroscopy. The derived Mössbauer parameter at room temperature clearly indicated the presence of Fe3+ ions in tetrahedral lattice sites. The catalytic activity of ferrisilicate was tested for the oxidation of CO with O2 at 673 K and was compared with the activities of iron-oxide-impregnated silicalite (FeOx/Sil) and Fe ion-exchanged ZSM-5 (FeZSM-5). The CO oxidation activity of the tetrahedrally coordinated Fe3+ in ferrisilicate was much lower than that of octahedrally coordinated Fe3+ in FeOx/Sil and Fe3+ in ion-exchange sites of FeZSM-5. Kinetic studies were performed on these catalysts at 623 K. On ferrisilicate, the reaction orders for CO and O2 were 1.0 and 1.1, respectively, while on FeOx and FeZSM-5 the reaction orders were 1.3 and 1.2 for CO, respectively, and near zero for O2 in both cases. For CO oxidation, both the activity and reaction mechanism on ferrisilicate differed markedly from those on FeOx/Sil and FeZSM-5. © 1993.

DOI： 10.1016/0927-6513(93)80078-9

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Event date： 2024.9.13

Language：Japanese   Presentation type：Oral presentation (general)  

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Event date： 2023.11.26 - 2023.11.29

Language：English   Presentation type：Oral presentation (invited, special)  

File： ACS2023_Paper_Azhar Uddin1.pdf

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Event date： 2023.9.26 - 2023.9.28

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Event date： 2023.9.11 - 2023.9.13

Language：Japanese   Presentation type：Oral presentation (general)  

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