A series of the Pt-Sn/SBA-15 catalysts were prepared and their properties characterized by using X-ray powder diffraction （XRD）, N2 adsorption-desorption, high resolution transmission electron microscope, X-ray phot...A series of the Pt-Sn/SBA-15 catalysts were prepared and their properties characterized by using X-ray powder diffraction （XRD）, N2 adsorption-desorption, high resolution transmission electron microscope, X-ray photoelectron spectroscopy （XPS） and H2-temperature programmed reduction. Their performances in long chain alkane dehydrogenation were evaluated in a fixed-bed microreactor with dodecane as a model alkane. The results indicated that SBA-15 maintained the well-order mesoporous structure during the reaction. The performance of the catalyst was found not dominated by its textural properties, but by the molar ratio of Sn to Pt which governed the degree of Sn reduction. Owing to the highest degree of Sn reduction, 1% （by mass） Pt-1.8% （by mass） Sn/SBA-15 showed the best catalytic activity. At 0.1 MPa and 470℃, the molar ratio of hydrogen to alkane at 4, and liquid hourly space velocity （LHSV） 20 h^-1, the dodecane conversion is 10%, and the dodecene selectivity is about 70%.展开更多
PtSnNaGa/ZSM-5 catalysts with different contents of Ga were prepared and characterized by X-ray diffraction (XRD), nitrogen adsorption, hydrogen chemisorption, ammonia temperature-programmed desorption (NH3-TPD), hydr...PtSnNaGa/ZSM-5 catalysts with different contents of Ga were prepared and characterized by X-ray diffraction (XRD), nitrogen adsorption, hydrogen chemisorption, ammonia temperature-programmed desorption (NH3-TPD), hydrogen temperature-programmed reduction (H2-TPR), and temperature-programmed oxidation (TPO) techniques. The performances of these catalysts for propane dehydrogenation were investigated. The test results indicated that the addition of Ga not only could improve the catalytic stability and propene selectivity, but also could effectively prevent the catalysts from coking. It was found that the PtSnNaGa(0.5 m%)/ZSM-5 catalyst exhibited the best performance in terms of propene selectivity and propane conversion. The high catalytic performance was most probably attributed to the presence of Ga that could strength- en the interaction between metals and the support to stabilize the catalytic active sites.展开更多
The alumina-modified SBA-15 （A12OJSBA-15） zeolite was prepared in a non-aqueous system by using toluene as the solvent, and was used to support the PtSn-based catalyst for propane dehydrogenation. The BET surface ar...The alumina-modified SBA-15 （A12OJSBA-15） zeolite was prepared in a non-aqueous system by using toluene as the solvent, and was used to support the PtSn-based catalyst for propane dehydrogenation. The BET surface area mea- surements, hydrogen chemisorption, FT-IR spectroscopy, NH3-TPD, XPS and TPO techniques were used to characterize the catalysts. Test results showed that the addition of alumina not only could modify the acid function of the support but also the structure of the metallic phase, thus affecting their catalytic properties. Among these catalysts studied, the PtSn/AI203 （5%）/ SBA-15 catalyst exhibited a best catalytic performance in terms of propane conversion and selectivity to propene. The high catalytic performance might be attributed to the relatively good Pt metal dispersion and/or the strong interaction between Pt and Sn species.展开更多
PtSnSr/HZSM-5 catalysts with different amounts of strontium were prepared by sequential impregnation method, and characterized by BET analysis, TEM, NH3-TPD, Hz-TPR, TPO and TG techniques. The results showed that the ...PtSnSr/HZSM-5 catalysts with different amounts of strontium were prepared by sequential impregnation method, and characterized by BET analysis, TEM, NH3-TPD, Hz-TPR, TPO and TG techniques. The results showed that the addition of strontium could modify the characteristics and properties of both acid function and metal function of Pt-Sn-based cata- lysts. In this case, PtSnSr/HZSM-5 catalyst with an appropriate amount of Sr （1.2%） showed higher catalytic activity and lower amount of coke deposits than PtSn/HZSM-5 catalyst. However, excessive loading of Sr could facilitate the reduction of Sn, which was unfavorable to the reaction. Afterwards, 1.0 m% of Na was added into the PtSnSr（1.2%）/HZSM-5 catalyst to improve the catalytic performance in propane dehydrogenation, and this catalyst displayed the best catalytic performance during our experiments. After having been subjected to reaction for 5 h, the PtSnNa（1.0%）Sr（1,2%）/HZSM-5 catalyst had achieved a higher than 95% selectivity towards propene along with a corresponding propane conversion rate of 32.2%.展开更多
The influence of mischmetal addition on physicochcmical properties of PtSnNa/ZSM-5 catalyst was studied by means of XRF, H2 chemisorption, XRD, TPR, NH3-TPD and TPO techniques. The results showed that the presence of ...The influence of mischmetal addition on physicochcmical properties of PtSnNa/ZSM-5 catalyst was studied by means of XRF, H2 chemisorption, XRD, TPR, NH3-TPD and TPO techniques. The results showed that the presence of mischmetal had an obvious impact on the catalytic performance of the PtSnNa/ZSM-5 catalyst. A suitable content of mischmetal not only could enhance the interactions between Pt species and the support, but also inhibit the formation of coke during the reaction, thus improving the catalytic activity and stability. In our experiments, when the content of mischmetal was 3m%, the catalyst exhibited best catalytic performance. However, the continuous addition of mischmetal could promote the reduction of Sn species to metallic tin, which was disadvantageous to the reaction.展开更多
The porous material ATZ with micro-mesopore hierarchical porosity was prepared by alkali treatment of parent HZSM-5 zeolite and applied for propane dehydrogenation. The zeolite samples were characterized by XRD, N2- p...The porous material ATZ with micro-mesopore hierarchical porosity was prepared by alkali treatment of parent HZSM-5 zeolite and applied for propane dehydrogenation. The zeolite samples were characterized by XRD, N2- physisorption, and NH3-TPD analysis. The results showed that the alkali treatment can modify the physicochemical prop- erties of HZSM-5 zeolite. In this case, the porous material ATZ showed larger extemal surface area with less acid sites as compared to the HZSM-5 zeolite. It was found out that the alkali treatment of HZSM-5 zeolite could promote the catalytic performance of PtSn/ATZ catalyst. The possible reason was ascribed to the low acidity of ATZ. Furthermore, the presence of mesopores could reduce the carbon deposits on the metallic surface, which was also favorable for the dehydrogenation reaction.展开更多
A series of B-Ni2P/SBA-15/cord monolithic catalysts were prepared by coating the slurry of the B-Ni2P/SBA-15 precursors on a pretreated cordierite support, and followed by temperature-programmed reduction in a H2 flow...A series of B-Ni2P/SBA-15/cord monolithic catalysts were prepared by coating the slurry of the B-Ni2P/SBA-15 precursors on a pretreated cordierite support, and followed by temperature-programmed reduction in a H2 flow. The samples were characterized by X-ray diffraction （XRD） and N2 adsorption-desorption technique. The catalytic activities for the hydrodesulfurization （HDS） of dibenzothiophene （DBT） were evaluated. The results showed that Ni2P phase was present in all B-Ni2P/SBA-1 5/cord monolithic catalysts. The specific surface areas （SBET） of the B-Ni2P/SBA-15/cord monolithic catalysts was first increased to 167 m2· g-1, and then decreased to 155 m2· g-1 with the increase of boron contents. The catalytic activity also showed the similar trend with the increase of boron contents. The 1.75% （by mass） B-Ni2P/SBA-15/cord monolithic catalysts exhibited the highest DBT conversion of 98.4% at 380 ℃. The cordierite-based monolithic catalysts showed better low temperature sensitivity for HDS of DBT in comparison with the particle catalysts. Moreover, two HDS routes, direct desulfurization （DDS） and hydrogenation （HYD）, proceeded independently over B-Ni2P/SBA-15/cord monolithic catalysts and the main pathway was DDS.展开更多
The design of non-noble metal heterogeneous catalyst with superior performance for selective hydrogenation or transfer hydrogenation of nitroarenes to amines is significant but challenging.Herein,a single-atom Fe supp...The design of non-noble metal heterogeneous catalyst with superior performance for selective hydrogenation or transfer hydrogenation of nitroarenes to amines is significant but challenging.Herein,a single-atom Fe supported by nitrogen-doped carbon(Fe_(1)/N-C)catalyst is reported.The Fe_(1)/N-C sample shows superior performances for the selective hydrogenation and transfer hydrogenation of nitrobenzene to aniline at different temperatures.Density functional theory(DFT)calculations show that the superior catalytic activity for the selective hydrogenation at lower temperatures could be attributed to the effective activation of the reactant and intermediates by the Fe_(1)/N-C.Moreover,the excellent performance of Fe_(1)/N-C for the selective transfer hydrogenation could be attributed to that the reaction energy barrier for dehydrogenation of isopropanol can be overcome by elevated temperatures.展开更多
Fenton reaction based on Fe2+-H2O2 system has been widely applied in water remediation, but the obvious drawbacks largely hinder its practical uses. Alternatively, heterogeneous nanomaterials with proper surface modif...Fenton reaction based on Fe2+-H2O2 system has been widely applied in water remediation, but the obvious drawbacks largely hinder its practical uses. Alternatively, heterogeneous nanomaterials with proper surface modification could be used as Fenton-like catalysts. Surface doping of Ti O2 could concentrate the pollutants surrounding the Fe3O4 catalyst, which might benefit the catalytic performance of Fe3O4. Herein, we reported that Ti O2-doped Fe3O4 nanoparticles(NPs) could be used as high-performance Fenton-like catalyst for dye decoloration in near neutral environment, where the doping of Ti O2 on Fe3O4 surface dramatically improved the catalytic activity of Fe3O4 in Fenton-like reaction. Ti O2-doped Fe3O4 NPs catalyzed the decomposition of H2O2 to oxidize methylene blue without external energy supply, resulting in effective decoloration. Ti O2-doped Fe3O4 NPs showed high catalytic activity under various p H values and even in the presence of radical scavenger. More catalysts and H2O2 would facilitate the decoloration. At higher temperature, the decoloration became faster and more effective. The implication to the environmental applications of Ti O2-doped Fe3O4 NPs is discussed.展开更多
基金Supported by the National Natural Science Foundation of China （20376005）.
文摘A series of the Pt-Sn/SBA-15 catalysts were prepared and their properties characterized by using X-ray powder diffraction （XRD）, N2 adsorption-desorption, high resolution transmission electron microscope, X-ray photoelectron spectroscopy （XPS） and H2-temperature programmed reduction. Their performances in long chain alkane dehydrogenation were evaluated in a fixed-bed microreactor with dodecane as a model alkane. The results indicated that SBA-15 maintained the well-order mesoporous structure during the reaction. The performance of the catalyst was found not dominated by its textural properties, but by the molar ratio of Sn to Pt which governed the degree of Sn reduction. Owing to the highest degree of Sn reduction, 1% （by mass） Pt-1.8% （by mass） Sn/SBA-15 showed the best catalytic activity. At 0.1 MPa and 470℃, the molar ratio of hydrogen to alkane at 4, and liquid hourly space velocity （LHSV） 20 h^-1, the dodecane conversion is 10%, and the dodecene selectivity is about 70%.
基金supports provided by the Production and Research Prospective Joint Research Project (BY2009153)the Science and Technology Support Program (BE2008129)of jiansu Province of chinathe National Natural Science Foundation of China(50873026)
文摘PtSnNaGa/ZSM-5 catalysts with different contents of Ga were prepared and characterized by X-ray diffraction (XRD), nitrogen adsorption, hydrogen chemisorption, ammonia temperature-programmed desorption (NH3-TPD), hydrogen temperature-programmed reduction (H2-TPR), and temperature-programmed oxidation (TPO) techniques. The performances of these catalysts for propane dehydrogenation were investigated. The test results indicated that the addition of Ga not only could improve the catalytic stability and propene selectivity, but also could effectively prevent the catalysts from coking. It was found that the PtSnNaGa(0.5 m%)/ZSM-5 catalyst exhibited the best performance in terms of propene selectivity and propane conversion. The high catalytic performance was most probably attributed to the presence of Ga that could strength- en the interaction between metals and the support to stabilize the catalytic active sites.
基金the National Nature Science Foundation of China (50873026, 21106017)the Production and Research Prospective Joint Research Project (BY2009153)+1 种基金the Science and Technology Support Program (BE2008129) of Jiangsu Province of Chinathe Specialized Research Fund for the Doctoral Program of Higher Education of China (20100092120047) for financial supports
文摘The alumina-modified SBA-15 （A12OJSBA-15） zeolite was prepared in a non-aqueous system by using toluene as the solvent, and was used to support the PtSn-based catalyst for propane dehydrogenation. The BET surface area mea- surements, hydrogen chemisorption, FT-IR spectroscopy, NH3-TPD, XPS and TPO techniques were used to characterize the catalysts. Test results showed that the addition of alumina not only could modify the acid function of the support but also the structure of the metallic phase, thus affecting their catalytic properties. Among these catalysts studied, the PtSn/AI203 （5%）/ SBA-15 catalyst exhibited a best catalytic performance in terms of propane conversion and selectivity to propene. The high catalytic performance might be attributed to the relatively good Pt metal dispersion and/or the strong interaction between Pt and Sn species.
基金The Production and Research Prospective Joint Research Project (BY2009153)The Science and Technology Support Program (BE2008129) of Jiangsu Province of Chinathe National Nature Science Foundation of China (50873026,21106017) for financial support
文摘PtSnSr/HZSM-5 catalysts with different amounts of strontium were prepared by sequential impregnation method, and characterized by BET analysis, TEM, NH3-TPD, Hz-TPR, TPO and TG techniques. The results showed that the addition of strontium could modify the characteristics and properties of both acid function and metal function of Pt-Sn-based cata- lysts. In this case, PtSnSr/HZSM-5 catalyst with an appropriate amount of Sr （1.2%） showed higher catalytic activity and lower amount of coke deposits than PtSn/HZSM-5 catalyst. However, excessive loading of Sr could facilitate the reduction of Sn, which was unfavorable to the reaction. Afterwards, 1.0 m% of Na was added into the PtSnSr（1.2%）/HZSM-5 catalyst to improve the catalytic performance in propane dehydrogenation, and this catalyst displayed the best catalytic performance during our experiments. After having been subjected to reaction for 5 h, the PtSnNa（1.0%）Sr（1,2%）/HZSM-5 catalyst had achieved a higher than 95% selectivity towards propene along with a corresponding propane conversion rate of 32.2%.
基金the Specialized Research Fund for the Doctoral Program of Higher Education of China (No.20100092120047)the Production and Research Prospective Joint Research Project (No.BY2009153)the National Nature Science Foundation of China (No.50873026) for financial supports
文摘The influence of mischmetal addition on physicochcmical properties of PtSnNa/ZSM-5 catalyst was studied by means of XRF, H2 chemisorption, XRD, TPR, NH3-TPD and TPO techniques. The results showed that the presence of mischmetal had an obvious impact on the catalytic performance of the PtSnNa/ZSM-5 catalyst. A suitable content of mischmetal not only could enhance the interactions between Pt species and the support, but also inhibit the formation of coke during the reaction, thus improving the catalytic activity and stability. In our experiments, when the content of mischmetal was 3m%, the catalyst exhibited best catalytic performance. However, the continuous addition of mischmetal could promote the reduction of Sn species to metallic tin, which was disadvantageous to the reaction.
基金the Production and Research Prospective Joint Research Project(BY2009153)Science and the National Nature Science Foundation of China(50873026,21106017)for financial supportthe Specialized Research Fund for the Doctoral Program of Higher Education of China(20100092120047)
文摘The porous material ATZ with micro-mesopore hierarchical porosity was prepared by alkali treatment of parent HZSM-5 zeolite and applied for propane dehydrogenation. The zeolite samples were characterized by XRD, N2- physisorption, and NH3-TPD analysis. The results showed that the alkali treatment can modify the physicochemical prop- erties of HZSM-5 zeolite. In this case, the porous material ATZ showed larger extemal surface area with less acid sites as compared to the HZSM-5 zeolite. It was found out that the alkali treatment of HZSM-5 zeolite could promote the catalytic performance of PtSn/ATZ catalyst. The possible reason was ascribed to the low acidity of ATZ. Furthermore, the presence of mesopores could reduce the carbon deposits on the metallic surface, which was also favorable for the dehydrogenation reaction.
基金Supported by the National Basic Research Program of China(2006CB202503)the Science Foundation of PetroChina(2010D-5006-0401)
文摘A series of B-Ni2P/SBA-15/cord monolithic catalysts were prepared by coating the slurry of the B-Ni2P/SBA-15 precursors on a pretreated cordierite support, and followed by temperature-programmed reduction in a H2 flow. The samples were characterized by X-ray diffraction （XRD） and N2 adsorption-desorption technique. The catalytic activities for the hydrodesulfurization （HDS） of dibenzothiophene （DBT） were evaluated. The results showed that Ni2P phase was present in all B-Ni2P/SBA-1 5/cord monolithic catalysts. The specific surface areas （SBET） of the B-Ni2P/SBA-15/cord monolithic catalysts was first increased to 167 m2· g-1, and then decreased to 155 m2· g-1 with the increase of boron contents. The catalytic activity also showed the similar trend with the increase of boron contents. The 1.75% （by mass） B-Ni2P/SBA-15/cord monolithic catalysts exhibited the highest DBT conversion of 98.4% at 380 ℃. The cordierite-based monolithic catalysts showed better low temperature sensitivity for HDS of DBT in comparison with the particle catalysts. Moreover, two HDS routes, direct desulfurization （DDS） and hydrogenation （HYD）, proceeded independently over B-Ni2P/SBA-15/cord monolithic catalysts and the main pathway was DDS.
基金the National Key R&D Program of China(2018YFA0702003)the National Natural Science Foundation of China(21890383,21671117,21871159 and21901135)the Science and Technology Key Project of Guangdong Province of China(2020B010188002)。
文摘The design of non-noble metal heterogeneous catalyst with superior performance for selective hydrogenation or transfer hydrogenation of nitroarenes to amines is significant but challenging.Herein,a single-atom Fe supported by nitrogen-doped carbon(Fe_(1)/N-C)catalyst is reported.The Fe_(1)/N-C sample shows superior performances for the selective hydrogenation and transfer hydrogenation of nitrobenzene to aniline at different temperatures.Density functional theory(DFT)calculations show that the superior catalytic activity for the selective hydrogenation at lower temperatures could be attributed to the effective activation of the reactant and intermediates by the Fe_(1)/N-C.Moreover,the excellent performance of Fe_(1)/N-C for the selective transfer hydrogenation could be attributed to that the reaction energy barrier for dehydrogenation of isopropanol can be overcome by elevated temperatures.
基金supported by the National Natural Science Foundation of China(Grant Nos.21307101 and 21301015)the Science & Technology Department of Sichuan Province(Pillar Program)(Grant No.2013FZ0060)+1 种基金Education Department of Sichuan Province(Grant No.15ZA0392)the Project of Postgraduate Degree Construction,Southwest University for Nationalities(Grant No.2015XWD-S0703)
文摘Fenton reaction based on Fe2+-H2O2 system has been widely applied in water remediation, but the obvious drawbacks largely hinder its practical uses. Alternatively, heterogeneous nanomaterials with proper surface modification could be used as Fenton-like catalysts. Surface doping of Ti O2 could concentrate the pollutants surrounding the Fe3O4 catalyst, which might benefit the catalytic performance of Fe3O4. Herein, we reported that Ti O2-doped Fe3O4 nanoparticles(NPs) could be used as high-performance Fenton-like catalyst for dye decoloration in near neutral environment, where the doping of Ti O2 on Fe3O4 surface dramatically improved the catalytic activity of Fe3O4 in Fenton-like reaction. Ti O2-doped Fe3O4 NPs catalyzed the decomposition of H2O2 to oxidize methylene blue without external energy supply, resulting in effective decoloration. Ti O2-doped Fe3O4 NPs showed high catalytic activity under various p H values and even in the presence of radical scavenger. More catalysts and H2O2 would facilitate the decoloration. At higher temperature, the decoloration became faster and more effective. The implication to the environmental applications of Ti O2-doped Fe3O4 NPs is discussed.
