The aromatization of light alkenes in liquefied petroleum gas (LPG) with and without dimethyl ether (DME) addition in the feed was investigated on a modified ZSM-5 catalyst.The results showed that under the given reac...The aromatization of light alkenes in liquefied petroleum gas (LPG) with and without dimethyl ether (DME) addition in the feed was investigated on a modified ZSM-5 catalyst.The results showed that under the given reaction conditions the selectivity of alkenes to high-octane gasoline blending components was markedly enhanced and the formation of propane and butanes was greatly suppressed with the addition of DME.It was also found that the distribution of C5+ components was changed a lot with DME addition into the LPG feed.The formation of branched hydrocarbons (mainly C6 C8 i-paraffin) and multi-methyl substituted aromatics,which are high octane number gasoline blending components,was promoted significantly,while the content of n-paraffins and olefins in C5+ components was decreased obviously,indicating that in addition to the oligomerization,cracking,hydrogen-transfer and dehydrogenation-cyclization of alkenes,the methylation of the formed aromatics and olefins intermediates also plays an important role in determining the product distribution due to the high reactivity of surface methoxy groups formed by DME.And this process,in combination with the syngas-to-methanol/DME technology,provides an alternative way to the production of high-octane gasoline from coal,natural gas or renewable raw materials.展开更多
The effect of dimethyl ether (DME) co-feed on the catalytic performance of methane dehy-droaromatization (MDA) over 6Mo/HZSM-5 catalyst was investigated as a function of DME concentration under reaction conditions of ...The effect of dimethyl ether (DME) co-feed on the catalytic performance of methane dehy-droaromatization (MDA) over 6Mo/HZSM-5 catalyst was investigated as a function of DME concentration under reaction conditions of T=1023 K, p=101 kPa and SV=1500 ml/(g·h). A high benzene yield was obtained and the stability of the catalyst was improved by adding 1.5%DME to the CH4 feed. The C6H6 yield was as high as ca. 10% even after reaction for 6 h. The stability of the catalyst was further improved when DME concentration in the co-feed gas was increased to an appropriate value. TGA and TPO results of the used 6Mo/HZSM-5 catalyst showed that the amount of coke on the used catalyst was reduced and the chemical nature of the coke was changed. When 1.5%DME was added to the CH4 feed, the coke formed on the catalyst could be burned off more easily than that when only CH4 was used as reactant. It is supposed that the oxygen in DME may play a role in preventing the coke burnt off at lower temperature from transforming into the coke burnt off at higher temperature, which results in the improvement of the stability of the catalyst.展开更多
The effect of temperature and hydrogen addition on undesired carbonaceous deposit formation during methane coupling was studied in DBD-plasma catalytic-wall reactors with Pd/Al2 O3, using electrical power to drive the...The effect of temperature and hydrogen addition on undesired carbonaceous deposit formation during methane coupling was studied in DBD-plasma catalytic-wall reactors with Pd/Al2 O3, using electrical power to drive the reaction.Experiments with thin catalyst layers allowed comparison of the performance of empty reactors and catalytic wall reactors without significantly influencing the plasma properties.The product distribution varies strongly in the temperature window between 25 and 200℃Minimal formation of deposits is found at an optimal temperature around 75℃ in the catalytic-wall reactors.The selectivity to deposits was c.a.10% with only 9 mg of catalyst loading instead of 45% in the blank reactor,while decreasing methane conversion only mildly.Co-feeding H2 to an empty reactor causes a similar decrease in selectivity to deposits,but in this case methane conversion also decreased significantly.Suppression of deposits formation in the catalytic-wall reactor at 75℃ is due to catalytic hydrogenation of mainly acetylene to ethylene.In the empty reactor,H2 co-feed decreases conversion but does not change the product distribution.The catalytic-wall reactors can be regenerated with H2-plasma at room temperature,which produces more added-value hydrocarbons.展开更多
基金supported by the "Action Plan of CAS to Support China’s New and Strategic Industries with Science and Technology(2012-2014)"the "Knowledge Innovation Program of the Chinese Academy of Sciences(S201041)""Youth Innovation Promotion Association CAS(2012-2015)"
文摘The aromatization of light alkenes in liquefied petroleum gas (LPG) with and without dimethyl ether (DME) addition in the feed was investigated on a modified ZSM-5 catalyst.The results showed that under the given reaction conditions the selectivity of alkenes to high-octane gasoline blending components was markedly enhanced and the formation of propane and butanes was greatly suppressed with the addition of DME.It was also found that the distribution of C5+ components was changed a lot with DME addition into the LPG feed.The formation of branched hydrocarbons (mainly C6 C8 i-paraffin) and multi-methyl substituted aromatics,which are high octane number gasoline blending components,was promoted significantly,while the content of n-paraffins and olefins in C5+ components was decreased obviously,indicating that in addition to the oligomerization,cracking,hydrogen-transfer and dehydrogenation-cyclization of alkenes,the methylation of the formed aromatics and olefins intermediates also plays an important role in determining the product distribution due to the high reactivity of surface methoxy groups formed by DME.And this process,in combination with the syngas-to-methanol/DME technology,provides an alternative way to the production of high-octane gasoline from coal,natural gas or renewable raw materials.
基金Financial supports from the Ministry of Science and Technology of Chinathe Natural Science Foundation of China+1 种基金the Chinese Academy of Sciencethe BP-China Joint Research Center are gratefully acknowledged.
文摘The effect of dimethyl ether (DME) co-feed on the catalytic performance of methane dehy-droaromatization (MDA) over 6Mo/HZSM-5 catalyst was investigated as a function of DME concentration under reaction conditions of T=1023 K, p=101 kPa and SV=1500 ml/(g·h). A high benzene yield was obtained and the stability of the catalyst was improved by adding 1.5%DME to the CH4 feed. The C6H6 yield was as high as ca. 10% even after reaction for 6 h. The stability of the catalyst was further improved when DME concentration in the co-feed gas was increased to an appropriate value. TGA and TPO results of the used 6Mo/HZSM-5 catalyst showed that the amount of coke on the used catalyst was reduced and the chemical nature of the coke was changed. When 1.5%DME was added to the CH4 feed, the coke formed on the catalyst could be burned off more easily than that when only CH4 was used as reactant. It is supposed that the oxygen in DME may play a role in preventing the coke burnt off at lower temperature from transforming into the coke burnt off at higher temperature, which results in the improvement of the stability of the catalyst.
基金supported by the Innovation Fund for Chemistry of NWO,grant number 731.014.303by SASOL。
文摘The effect of temperature and hydrogen addition on undesired carbonaceous deposit formation during methane coupling was studied in DBD-plasma catalytic-wall reactors with Pd/Al2 O3, using electrical power to drive the reaction.Experiments with thin catalyst layers allowed comparison of the performance of empty reactors and catalytic wall reactors without significantly influencing the plasma properties.The product distribution varies strongly in the temperature window between 25 and 200℃Minimal formation of deposits is found at an optimal temperature around 75℃ in the catalytic-wall reactors.The selectivity to deposits was c.a.10% with only 9 mg of catalyst loading instead of 45% in the blank reactor,while decreasing methane conversion only mildly.Co-feeding H2 to an empty reactor causes a similar decrease in selectivity to deposits,but in this case methane conversion also decreased significantly.Suppression of deposits formation in the catalytic-wall reactor at 75℃ is due to catalytic hydrogenation of mainly acetylene to ethylene.In the empty reactor,H2 co-feed decreases conversion but does not change the product distribution.The catalytic-wall reactors can be regenerated with H2-plasma at room temperature,which produces more added-value hydrocarbons.