The isomerization of n-pentane to generate high-quality blending components for clean gasoline was catalyzed by several amide-AlCl3-based ionic liquid(IL) analogs with various amides as donor molecules. The catalytic ...The isomerization of n-pentane to generate high-quality blending components for clean gasoline was catalyzed by several amide-AlCl3-based ionic liquid(IL) analogs with various amides as donor molecules. The catalytic performance of these IL analogs was evaluated in a magnetic agitated autoclave operated in batch mode.IL analog based n-methylacetamide(NMA)-AlCl3 with the amide/AlCl3 molar ratio of 0.65 showed excellent performance toward n-pentane isomerization because 0.65 NMA-1.0 AlCl3 had a low viscosity and bidentate coordination structure. The influences of reaction time, reaction temperature, and stirring speed on the catalytic performance were also investigated. Optimal reaction conditions comprised the reaction time of 1 h, the reaction temperature of 40 °C, and the stirring speed of 1500 r·min-1. Under optimal condition, the n-C5 conversion,research octane number(RON) increment, total liquids yield, and isoparaffin yield in isomerized oil were56.80%, 13.51, 89.90 wt%, and 44.32 wt%, respectively. A new mathematical model was constructed to predict the relationships among RON increment, RON increment/n-C5 conversion ratio, and n-C5 conversion. The new model indicated that an appropriate conversion per pass of n-C5 did not exceed 50%–55%. Various cycloparaffin additives were used to improve the catalytic performance of 0.65 NMA-1.0 AlCl3. The n-C5 conversion increased from 56.80% to 67.32%. The RON increment, total liquids yield, and isoparaffin yield reached 17.83, 97.36 wt%,and 63.74 wt%, respectively.展开更多
Isobutane alkylation with 2-butene to produce high-quality gasoline was catalyzed by Nmethylacetamide(NMA)-AlCl3 based ionic liquid(IL) analog with a NMA/AlCl3 molar ratio of 0.75 and CuCl modification,which was marke...Isobutane alkylation with 2-butene to produce high-quality gasoline was catalyzed by Nmethylacetamide(NMA)-AlCl3 based ionic liquid(IL) analog with a NMA/AlCl3 molar ratio of 0.75 and CuCl modification,which was marked as CuCl-modified 0.75 NMA-1.0 AlCl3.The long-term experiment was carried out in the autoclave operated in continuous mode to investigate the distribution of alkylate under different experimental nodes.The result indicated that the long-term alkylation was divided into three stages:rising,stable,and descending regions.C8 selectivity and molar ratio of trimethylpentanes(TMPs) to dimethylhexanes(DMHs) reached the highest level in the stable region,and research octane number(RON) of alkylate was as high as 97.Anionic Al species([AlbCl7]^-,[A1 CuC15]^-) and cationic Al species([AlCl2 L]^+) from IL analog as two active Lewis acidic species played a catalytic role in the long-term alkylation,whereas the neutral Al species did not participate into the alkylation.Moreover,the structure of CuCl-modified 0.75 NMA-1.0 AlCl3 was destroyed after the deactivation,and CuCl was enriched in the CD2 Cl2-insoluble substance,resulting in a decreasing TMP/DMH ratio.The catalytic lifetime of IL analog was similar with CuCl-modified 0.55 Et3 NHCl-1.0 AlCl3 IL,but IL analog had a lower cost.展开更多
The spectral structures of acetamide-AlCl_(3)-based ionic liquid(IL)analogs were determined in detail through IR,NMR,and Raman spectroscopy.IR spectroscopy showed that 0.65AA-1.0AlCl_(3) was the coordination structure...The spectral structures of acetamide-AlCl_(3)-based ionic liquid(IL)analogs were determined in detail through IR,NMR,and Raman spectroscopy.IR spectroscopy showed that 0.65AA-1.0AlCl_(3) was the coordination structure of Al and O atoms because of the resonance structure of acetamide.The mutual verification of the results of ^(27)Al NMR and ^(1)H NMR indicated that acetamide coexisted mainly in the form of cationic Al species and molecular Al species in xAA-1.0AlCl_(3),and AA/AlCl_(3) molar ratio affected the transformation of cationic Al species to molecular Al species.xAA-1.0AlCl_(3) was used as a green acidic catalyst for isobutene oligomerization,and the effects of AA/AlCl_(3) molar ratio,reaction temperature,reaction time,and volumetric ratio between IL analog and isobutene on product distribution were investigated.Optimal reaction conditions were AA/AlCl_(3) molar ratio of 0.75,reaction temperature of 60 C,reaction time of 30 min,and catalyst/i-C4¼volumetric ratio of 1.4 v/v.Under optimal conditions,isobutene conversion,(C8^(-)+C12^(-))selectivity,(C16^(-)+C20^(-))selectivity,and by-product selectivity were 85.26,80.20,6.80,and 13.00 wt%,respectively。展开更多
基金Supported by the National Natural Science Foundation of China(21802047)the Scientific Research Funds of Huaqiao University(600005-Z17Y0073).
文摘The isomerization of n-pentane to generate high-quality blending components for clean gasoline was catalyzed by several amide-AlCl3-based ionic liquid(IL) analogs with various amides as donor molecules. The catalytic performance of these IL analogs was evaluated in a magnetic agitated autoclave operated in batch mode.IL analog based n-methylacetamide(NMA)-AlCl3 with the amide/AlCl3 molar ratio of 0.65 showed excellent performance toward n-pentane isomerization because 0.65 NMA-1.0 AlCl3 had a low viscosity and bidentate coordination structure. The influences of reaction time, reaction temperature, and stirring speed on the catalytic performance were also investigated. Optimal reaction conditions comprised the reaction time of 1 h, the reaction temperature of 40 °C, and the stirring speed of 1500 r·min-1. Under optimal condition, the n-C5 conversion,research octane number(RON) increment, total liquids yield, and isoparaffin yield in isomerized oil were56.80%, 13.51, 89.90 wt%, and 44.32 wt%, respectively. A new mathematical model was constructed to predict the relationships among RON increment, RON increment/n-C5 conversion ratio, and n-C5 conversion. The new model indicated that an appropriate conversion per pass of n-C5 did not exceed 50%–55%. Various cycloparaffin additives were used to improve the catalytic performance of 0.65 NMA-1.0 AlCl3. The n-C5 conversion increased from 56.80% to 67.32%. The RON increment, total liquids yield, and isoparaffin yield reached 17.83, 97.36 wt%,and 63.74 wt%, respectively.
基金Supported by the National Natural Science Foundation of China(No.21802047)the Scientific Research Funds of Huaqiao University(No.600005-Z17Y0073)
文摘Isobutane alkylation with 2-butene to produce high-quality gasoline was catalyzed by Nmethylacetamide(NMA)-AlCl3 based ionic liquid(IL) analog with a NMA/AlCl3 molar ratio of 0.75 and CuCl modification,which was marked as CuCl-modified 0.75 NMA-1.0 AlCl3.The long-term experiment was carried out in the autoclave operated in continuous mode to investigate the distribution of alkylate under different experimental nodes.The result indicated that the long-term alkylation was divided into three stages:rising,stable,and descending regions.C8 selectivity and molar ratio of trimethylpentanes(TMPs) to dimethylhexanes(DMHs) reached the highest level in the stable region,and research octane number(RON) of alkylate was as high as 97.Anionic Al species([AlbCl7]^-,[A1 CuC15]^-) and cationic Al species([AlCl2 L]^+) from IL analog as two active Lewis acidic species played a catalytic role in the long-term alkylation,whereas the neutral Al species did not participate into the alkylation.Moreover,the structure of CuCl-modified 0.75 NMA-1.0 AlCl3 was destroyed after the deactivation,and CuCl was enriched in the CD2 Cl2-insoluble substance,resulting in a decreasing TMP/DMH ratio.The catalytic lifetime of IL analog was similar with CuCl-modified 0.55 Et3 NHCl-1.0 AlCl3 IL,but IL analog had a lower cost.
基金support of the National Natural Science Foundation of China(No.21802047)the Scientific Research Funds of Huaqiao University(No.600005-Z17Y0073),Xiamen,China.
文摘The spectral structures of acetamide-AlCl_(3)-based ionic liquid(IL)analogs were determined in detail through IR,NMR,and Raman spectroscopy.IR spectroscopy showed that 0.65AA-1.0AlCl_(3) was the coordination structure of Al and O atoms because of the resonance structure of acetamide.The mutual verification of the results of ^(27)Al NMR and ^(1)H NMR indicated that acetamide coexisted mainly in the form of cationic Al species and molecular Al species in xAA-1.0AlCl_(3),and AA/AlCl_(3) molar ratio affected the transformation of cationic Al species to molecular Al species.xAA-1.0AlCl_(3) was used as a green acidic catalyst for isobutene oligomerization,and the effects of AA/AlCl_(3) molar ratio,reaction temperature,reaction time,and volumetric ratio between IL analog and isobutene on product distribution were investigated.Optimal reaction conditions were AA/AlCl_(3) molar ratio of 0.75,reaction temperature of 60 C,reaction time of 30 min,and catalyst/i-C4¼volumetric ratio of 1.4 v/v.Under optimal conditions,isobutene conversion,(C8^(-)+C12^(-))selectivity,(C16^(-)+C20^(-))selectivity,and by-product selectivity were 85.26,80.20,6.80,and 13.00 wt%,respectively。
基金supports from the National Natural Science Foundation of China (No.52004062)the Fundamental Research Funds for the Central Universities,China (No.N2125014).
