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01227 Partial oxidation of methane to synthesis gas over supported ruthenium catalysts
03 Partial oxidation cobalt-based catalysts
98fQ1224
of methane over nickel- and
Swaan. H. M. et al. Stud. Surf Sci. Caral.. 1997, 107, 447-453. Testinu of Co- and Ni-based catalvsts for the martial oxidation of methane to syngas at 600900°C was carried out. Cobalt catalysts were active for combustion of CH4 to COz, but showed a low selectivity to CO and Hz, unless promoted with elements which favoured Co reducibility. A mechanistic study was conducted using Ni/AlzOs catalyst as an active and selective material. A two-step process was proposed and a detailed description of the catalytic bed under reaction conditions is provided.
Partial oxidation of methane to syngas over NIloaded ultrastable HY zeollte catalysts
9Blo1225
Pena, M. A. et al. Stud. SutfSci. Catal., 1997, 107, 441-446. In the partial oxidation of methane to synthesis gas, N&containing HY zeolites are active. The activity of these zeolites was found to depend strongly on the Ni-loading. At low Ni-content where Ni was essentially ionexchanged, catalysts were thus almost inactive. Zeolites with high Ni contents, however, were very active. Results from TPR, CO chemisorption and XPS studies revealed that small clusters of Ni species formed on the zeolite act as catalytic centres for the reaction.
Gaseous fuels (derived gaseous fuels)
96lo1231 The production of synthesis gas by the redox of cerlum oxide Otsuka, K. et al. Stud. Swf Sci. Catal., 1997, The authors have studied the oxidation of CH4 gaseous oxygen and the subsequent reduction Rz by the reduced cerium oxide, CeOz_x, atmospheric pressure at 673 to 1073 K.
107, 531-536. with CeOs in the absence of of CO2 to CO or of RrO to have been studied under
9Blo1232 Pulse detonation device for coal gasification. Hunter, L. G., Jr. U.S. US 5,672,184 (Cl. 48-77; ClOJ3/70), 30 Sep 1997, US AUDI. 265.384. 24 Jun 1994. 12 DD. detonation device is kmpidyed in a coal gasification system to A discharge hot exhaust pulses into the gasifier. In addition, it discharges reverse flow pulses into a ceramic candle filter system to dislodge particulate build up on the candles. The pulse detonation device utilizes a rotatable core feed cylinder, which is carried within an inner side wall of the stationary annular detonation chamber. The core feed cylinder has ports in the side wall that register with ports in the inner side wall of the annular detonation chamber at least once each revolution. Valves mounted to the outer side wall of the annular detonation chamber introduce the fuel.
puik
Reactor and method for gasification of low-grade coal powder to obtain clean fuel-type gas
98JQ1233
96iQl226 Partial oxidation of methane to synthesis gas experimental and modelllng studles Hofstad, K. H. et al. Stud. Surf Sci. Catal., 1997, 107, 415-420. The partial oxidation of methane to synthesis gas has been studied in monolithic type catalysts containing Pt or Rh. The experiments were ‘carried out at 600-105o”C, 1 bar and space times in the range 0.001-0.040 s. Short space times were chosen in order to study the reaction at conditions far from equil. Pt-impregnated monoliths were less favourable for the production of synthesis gas. Separate studies of reverse water-gas shift and steam reforming at the same temperature and space times showed that the monoliths were active for these reactions. Simulations based on a model taken from the literature consisting of 19 elementary steps could fit the experimental data for the Pt catalyst. The measured axial temperature profiles of the reactor were included in the model.
Partial oxidation of methane to synthesis gas over supported ruthenium catalysts
9m1227
Boucouvalas. J. et al. Stud. Surf Sci. Catal., 1997, 107, 435-440. _ Usine Ru suooorted on SiO,. r--Al~hOa. YSZ.and TiO, catalvsts. the oartial oxidition of ‘methane to synthe&-‘gas has been- investigated in the temperature range of 550-750°C. The RufTiOr catalyst exhibits up to 65% selectivity to synthesis gas in the low methane-conversion range, whereas all other catalysts yield zero selectivity under similar conditions. Isotopic labelling experiments demonstrate that the direct partial oxidation route is largely responsible for the high CO and Hr selectivity at low methane conversions, observed over the Ru/TiOz catalyst.
Performance of Ni/La203 catalyst in carbon dioxlde 96lO1226 I reforming of methane to synthesis gas
Zhana, Z. and Vervkios, X. et al. Stud. SurfSci. Catal., 1997, 107,511-516. During the initial 2-5 h, the rate of carbon dioxide reforming of methane over a Ni/LazOj catalyst was found to increase and then tends to be invariable with time on stream. A kinetic isotopic study shows that the reaction rate is reduced, by a factor of 1.2-2.0 upon switching the reactant mixture mixture from CH&Oz to CDJCOz, suggesting that methane activation is a slow step. Chemisorptive studies indicate that a portion of the Ni surface is decorated with lanthanum species originating from the LazOs support, thus suppressing CO chemisorption and disproportionation. FTIR, XRD, XPS and SIMS mechanistic studies suggest that the interaction between nickel and lanthanum suecies creates a new tvoe of synergetic sites at the Ni-LazOs interfacial ‘area, which offer act&i and stable performance of carbon dioxide reforming of methane to synthesis gas over the stated catalyst.
Preparation of a natural gas substttute by hydro96lo1229 gaslflcation of coal Porada, S. Garbo-Energochemical-Ekol., 1996,41, (5), 186188. (In Polish) The hydrogasification process of a lignite and a gas-splint coal at nonisothermal conditions was studied. The conversion coefficient of carbon and yield of gaseous hydrocarbon have been calculated.
96/01230 Process and apparatus for coal gasification for high gas yield and removal of molten slag Ikeda, Y. et al. Jpn. Kokai Tokkyo Koho JP 09,202,887 [97,202,887] (Cl. ClOJ3/46), 5 Aug 1997, Appl. 96/11,465, 26 Jan 1996 5 pp. (In Japanese) Following the entrained gasification furnace, high-temperature Hz0 and COz in coal gas are treated by water gas reaction with carbon in a cokefilling shaft furnace to cool the gas and increase gas yield and fly slag and unburned char are collected by coke. The apparatus has a coke-filling shaft furnace with a supplier of coke and an exhauster of reacted coke, collected slag, and collected char. High-temperature coal gas can be cooled without slag deposition and HrO and COz in the gas can be efficiently converted to fuels using the heat of the gas.
Karpenko, E. I. et al. PCT Int. Appl. WG 97 25,391 (Cl. ClOJ3/18), 17 Jul 1997, Appl. 96/RU2, 3 Jan 1996, 13 pp. (In Russian) The process involves injecting powdered coal is into a reactor apparatus for gasification, using a part of the coal feed pre-treated in side chambers for beneficiation by a low-temperature plasma in the presence of Oz. The plasma pre-treatment stage includes a partial combustion of coal with Ox for preheating as well as decreased consumption of electrical power. The feed and beneficiated coal fractions are injected tangentially into the reactor along with superheated steam for gasification at nominally lOOo”C, to obtain an ecological clean fuel-type gas. The typical feed into reactor is the coal powder at 200 kg/h, plasma-treated coal powder at 130 kg/h and the superheated steam at 300 kg/h. This produces a synthesis gas containing COz 4.8, Hz 18.2, CO 19.1, and CH4 2.1% by volume.
96lO1234 modelllng
Recent progress in underground coal gasification
Coeme, A. et al. DGMK Tagungsber., 1997, 9703 (Proceedings ICCS ‘97, Volume 2). 1271-1274. Recent modelling works in Belgium are outlined. The models were developed in the framework of the two European Underground Coal Gasification (UCG) field trials at great depth: Thulin (Belgium), 1980-1987 and Alcorisa, 1992-1997.
96lO1235 Solar energ gasification of solid carbonaceous material in liquid dispersYon Epstein, M. U.S. US 5,647,877 (Cl. 48-210; ClOJ3/46), 15 Jd 1997, US Appl. 270,676, 22 Jun 1994, 9 pp. Solar energy was used for syngas production from carbonaceous material. An aqueous dispersion of carbonaceous material was injected into a reactor in the form of a shower or a jet of droplets, and the droplets are allowed to sink inside the reactor across a high-temperature focal zone. This zone was projected into the reactor by a system for the concentration of solar radiation. The residence time inside the reactor is adjustable by a countercurrent gas flow or by the injection of two or more discrete droplet jets in an impinging jet arrangement.
96lO1236 Steam gaslflcatlon of wheat straw, barley straw, willow and olaanteus ~“”
~~~~
Hansen, L. K. et al. Risoe Natl. Laboratory, [Rep.] Risoe-R, 1997, (RisoeR-944), 1-31. The Hz0 gasification char-reactivity of wheat straw, barley straw, willow and giganteus was performed in a pressurized thermogravimetric analyser. A total of 58 experiments were undertaken. A full account of the results is presented in the paper. The project has been carried out under the EFP-95 program for the Danish Ministry of Environment and Energy and for the Danish utility associations Elsam and Elkraft.
96lQ1237 S ngas production by partial oxidation of methane: dependence or reactivity on catalyst properties and contact time
Basini, L. et al. Stud. Surf&i. Catal., 1997, 107, 429-434. A study into the effects of very short contact times on molecular aspects of the reaction mechanism for the partial oxidation of methane with a rhodium catalyst. A fixed bed micro-reactor and a reaction chamber equipped for DRIFI and mass spectrometry was used. Small surface rhodium carbonvl clusters were selectively generated at contact times >2, while at shorter contact times these species were not present. Different catalytic activities and selectivities were observed.
98/01238 A Texas project Illustrates the benefits of integrated gasification Philcox, J. and Fenner, G. W. Oil Gas J., 1997, 95, (28), 41-44, 46. A natural gas-based complex in Texas City, Texas, is jointly owned and operated by Praxair Inc. and Texaco Inc.. The unit, which started up in June 1996, produces 50 MMcfd of syngas. In addition to the gasifier, the site includes a 1500 ton/day air separation unit and 42-MW cogeneration plant.
Fuel and Energy AbHracts
March 1998
109
98fQ1224
of methane over nickel- and
Swaan. H. M. et al. Stud. Surf Sci. Caral.. 1997, 107, 447-453. Testinu of Co- and Ni-based catalvsts for the martial oxidation of methane to syngas at 600900°C was carried out. Cobalt catalysts were active for combustion of CH4 to COz, but showed a low selectivity to CO and Hz, unless promoted with elements which favoured Co reducibility. A mechanistic study was conducted using Ni/AlzOs catalyst as an active and selective material. A two-step process was proposed and a detailed description of the catalytic bed under reaction conditions is provided.
Partial oxidation of methane to syngas over NIloaded ultrastable HY zeollte catalysts
9Blo1225
Pena, M. A. et al. Stud. SutfSci. Catal., 1997, 107, 441-446. In the partial oxidation of methane to synthesis gas, N&containing HY zeolites are active. The activity of these zeolites was found to depend strongly on the Ni-loading. At low Ni-content where Ni was essentially ionexchanged, catalysts were thus almost inactive. Zeolites with high Ni contents, however, were very active. Results from TPR, CO chemisorption and XPS studies revealed that small clusters of Ni species formed on the zeolite act as catalytic centres for the reaction.
Gaseous fuels (derived gaseous fuels)
96lo1231 The production of synthesis gas by the redox of cerlum oxide Otsuka, K. et al. Stud. Swf Sci. Catal., 1997, The authors have studied the oxidation of CH4 gaseous oxygen and the subsequent reduction Rz by the reduced cerium oxide, CeOz_x, atmospheric pressure at 673 to 1073 K.
107, 531-536. with CeOs in the absence of of CO2 to CO or of RrO to have been studied under
9Blo1232 Pulse detonation device for coal gasification. Hunter, L. G., Jr. U.S. US 5,672,184 (Cl. 48-77; ClOJ3/70), 30 Sep 1997, US AUDI. 265.384. 24 Jun 1994. 12 DD. detonation device is kmpidyed in a coal gasification system to A discharge hot exhaust pulses into the gasifier. In addition, it discharges reverse flow pulses into a ceramic candle filter system to dislodge particulate build up on the candles. The pulse detonation device utilizes a rotatable core feed cylinder, which is carried within an inner side wall of the stationary annular detonation chamber. The core feed cylinder has ports in the side wall that register with ports in the inner side wall of the annular detonation chamber at least once each revolution. Valves mounted to the outer side wall of the annular detonation chamber introduce the fuel.
puik
Reactor and method for gasification of low-grade coal powder to obtain clean fuel-type gas
98JQ1233
96iQl226 Partial oxidation of methane to synthesis gas experimental and modelllng studles Hofstad, K. H. et al. Stud. Surf Sci. Catal., 1997, 107, 415-420. The partial oxidation of methane to synthesis gas has been studied in monolithic type catalysts containing Pt or Rh. The experiments were ‘carried out at 600-105o”C, 1 bar and space times in the range 0.001-0.040 s. Short space times were chosen in order to study the reaction at conditions far from equil. Pt-impregnated monoliths were less favourable for the production of synthesis gas. Separate studies of reverse water-gas shift and steam reforming at the same temperature and space times showed that the monoliths were active for these reactions. Simulations based on a model taken from the literature consisting of 19 elementary steps could fit the experimental data for the Pt catalyst. The measured axial temperature profiles of the reactor were included in the model.
Partial oxidation of methane to synthesis gas over supported ruthenium catalysts
9m1227
Boucouvalas. J. et al. Stud. Surf Sci. Catal., 1997, 107, 435-440. _ Usine Ru suooorted on SiO,. r--Al~hOa. YSZ.and TiO, catalvsts. the oartial oxidition of ‘methane to synthe&-‘gas has been- investigated in the temperature range of 550-750°C. The RufTiOr catalyst exhibits up to 65% selectivity to synthesis gas in the low methane-conversion range, whereas all other catalysts yield zero selectivity under similar conditions. Isotopic labelling experiments demonstrate that the direct partial oxidation route is largely responsible for the high CO and Hr selectivity at low methane conversions, observed over the Ru/TiOz catalyst.
Performance of Ni/La203 catalyst in carbon dioxlde 96lO1226 I reforming of methane to synthesis gas
Zhana, Z. and Vervkios, X. et al. Stud. SurfSci. Catal., 1997, 107,511-516. During the initial 2-5 h, the rate of carbon dioxide reforming of methane over a Ni/LazOj catalyst was found to increase and then tends to be invariable with time on stream. A kinetic isotopic study shows that the reaction rate is reduced, by a factor of 1.2-2.0 upon switching the reactant mixture mixture from CH&Oz to CDJCOz, suggesting that methane activation is a slow step. Chemisorptive studies indicate that a portion of the Ni surface is decorated with lanthanum species originating from the LazOs support, thus suppressing CO chemisorption and disproportionation. FTIR, XRD, XPS and SIMS mechanistic studies suggest that the interaction between nickel and lanthanum suecies creates a new tvoe of synergetic sites at the Ni-LazOs interfacial ‘area, which offer act&i and stable performance of carbon dioxide reforming of methane to synthesis gas over the stated catalyst.
Preparation of a natural gas substttute by hydro96lo1229 gaslflcation of coal Porada, S. Garbo-Energochemical-Ekol., 1996,41, (5), 186188. (In Polish) The hydrogasification process of a lignite and a gas-splint coal at nonisothermal conditions was studied. The conversion coefficient of carbon and yield of gaseous hydrocarbon have been calculated.
96/01230 Process and apparatus for coal gasification for high gas yield and removal of molten slag Ikeda, Y. et al. Jpn. Kokai Tokkyo Koho JP 09,202,887 [97,202,887] (Cl. ClOJ3/46), 5 Aug 1997, Appl. 96/11,465, 26 Jan 1996 5 pp. (In Japanese) Following the entrained gasification furnace, high-temperature Hz0 and COz in coal gas are treated by water gas reaction with carbon in a cokefilling shaft furnace to cool the gas and increase gas yield and fly slag and unburned char are collected by coke. The apparatus has a coke-filling shaft furnace with a supplier of coke and an exhauster of reacted coke, collected slag, and collected char. High-temperature coal gas can be cooled without slag deposition and HrO and COz in the gas can be efficiently converted to fuels using the heat of the gas.
Karpenko, E. I. et al. PCT Int. Appl. WG 97 25,391 (Cl. ClOJ3/18), 17 Jul 1997, Appl. 96/RU2, 3 Jan 1996, 13 pp. (In Russian) The process involves injecting powdered coal is into a reactor apparatus for gasification, using a part of the coal feed pre-treated in side chambers for beneficiation by a low-temperature plasma in the presence of Oz. The plasma pre-treatment stage includes a partial combustion of coal with Ox for preheating as well as decreased consumption of electrical power. The feed and beneficiated coal fractions are injected tangentially into the reactor along with superheated steam for gasification at nominally lOOo”C, to obtain an ecological clean fuel-type gas. The typical feed into reactor is the coal powder at 200 kg/h, plasma-treated coal powder at 130 kg/h and the superheated steam at 300 kg/h. This produces a synthesis gas containing COz 4.8, Hz 18.2, CO 19.1, and CH4 2.1% by volume.
96lO1234 modelllng
Recent progress in underground coal gasification
Coeme, A. et al. DGMK Tagungsber., 1997, 9703 (Proceedings ICCS ‘97, Volume 2). 1271-1274. Recent modelling works in Belgium are outlined. The models were developed in the framework of the two European Underground Coal Gasification (UCG) field trials at great depth: Thulin (Belgium), 1980-1987 and Alcorisa, 1992-1997.
96lO1235 Solar energ gasification of solid carbonaceous material in liquid dispersYon Epstein, M. U.S. US 5,647,877 (Cl. 48-210; ClOJ3/46), 15 Jd 1997, US Appl. 270,676, 22 Jun 1994, 9 pp. Solar energy was used for syngas production from carbonaceous material. An aqueous dispersion of carbonaceous material was injected into a reactor in the form of a shower or a jet of droplets, and the droplets are allowed to sink inside the reactor across a high-temperature focal zone. This zone was projected into the reactor by a system for the concentration of solar radiation. The residence time inside the reactor is adjustable by a countercurrent gas flow or by the injection of two or more discrete droplet jets in an impinging jet arrangement.
96lO1236 Steam gaslflcatlon of wheat straw, barley straw, willow and olaanteus ~“”
~~~~
Hansen, L. K. et al. Risoe Natl. Laboratory, [Rep.] Risoe-R, 1997, (RisoeR-944), 1-31. The Hz0 gasification char-reactivity of wheat straw, barley straw, willow and giganteus was performed in a pressurized thermogravimetric analyser. A total of 58 experiments were undertaken. A full account of the results is presented in the paper. The project has been carried out under the EFP-95 program for the Danish Ministry of Environment and Energy and for the Danish utility associations Elsam and Elkraft.
96lQ1237 S ngas production by partial oxidation of methane: dependence or reactivity on catalyst properties and contact time
Basini, L. et al. Stud. Surf&i. Catal., 1997, 107, 429-434. A study into the effects of very short contact times on molecular aspects of the reaction mechanism for the partial oxidation of methane with a rhodium catalyst. A fixed bed micro-reactor and a reaction chamber equipped for DRIFI and mass spectrometry was used. Small surface rhodium carbonvl clusters were selectively generated at contact times >2, while at shorter contact times these species were not present. Different catalytic activities and selectivities were observed.
98/01238 A Texas project Illustrates the benefits of integrated gasification Philcox, J. and Fenner, G. W. Oil Gas J., 1997, 95, (28), 41-44, 46. A natural gas-based complex in Texas City, Texas, is jointly owned and operated by Praxair Inc. and Texaco Inc.. The unit, which started up in June 1996, produces 50 MMcfd of syngas. In addition to the gasifier, the site includes a 1500 ton/day air separation unit and 42-MW cogeneration plant.
Fuel and Energy AbHracts
March 1998
109