With ongoing global warming and increasing energy demands,the CH_(4)-CO_(2)reforming reaction(dry reforming of methane,DRM)has garnered significant attention as a promising carbon capture and utilization technology.Ni...With ongoing global warming and increasing energy demands,the CH_(4)-CO_(2)reforming reaction(dry reforming of methane,DRM)has garnered significant attention as a promising carbon capture and utilization technology.Nickel-based catalysts are renowned for their outstanding activity and selectivity in this process.The impact of metal-support interaction(MSI),on Ni-based catalyst performance has been extensively researched and debated recently.This paper reviews the recent research progress of MSI on Ni-based catalysts and their characterization and modulation strategies in catalytic reactions.From the perspective of MSI,the effects of different carriers(metal oxides,carbon materials and molecular sieves,etc.)are introduced on the dispersion and surface structure of Ni active metal particles,and the effect of MSI on the activity and stability of DRM reactions on Ni-based catalysts is discussed in detail.Future research should focus on better understanding and controlling MSI to improve the performance and durability of nickel-based catalysts in CH_(4)-CO_(2)reforming,advancing cleaner energy technologies.展开更多
Nickel and nickel-ceria catalysts supported on high surface area silica, with 6 wt% Ni and 20 wt% CeO2 were prepared by microwave assisted(co) precipitation method. The catalysts were investigated by XRD,TPR and XPS a...Nickel and nickel-ceria catalysts supported on high surface area silica, with 6 wt% Ni and 20 wt% CeO2 were prepared by microwave assisted(co) precipitation method. The catalysts were investigated by XRD,TPR and XPS analyses and they were tested in partial oxidation of methane(CPO). The catalytic reaction was carried out at atmospheric pressure in a temperature range of 400–800℃ with a feed gas mixture containing methane and oxygen in a molecular ratio CH4/O2=2. The Ni catalyst exhibited 60% methane conversion with 60% selectivity to CO already at 500℃. On the contrary, the Ni–Ce catalyst was inert to CPO up to 700℃. Moreover, the former catalyst reproduced its activity at the descending temperatures maintaining a good stability at 600℃, over a reaction time of 80 h, whereas the latter one completely deactivated. Test of CH4 temperature programmed surface reaction(CH4-TPSR) revealed a higher methane activation temperature(> 100℃) for the Ni–Ce catalyst as compared to the Ni one. Noticeable improvement of the ceria containing catalyst occurred when the reaction test started at a temperature higher than the methane decomposition temperature. In this case, the sample achieved the same catalytic behavior of the Ni catalyst. As confirmed by XPS analyses, the distinct electronic state of the supported nickel was responsible for the differences in catalytic behavior.展开更多
The SiO2-Supported (PPh3)2HPt(μ-CO) (μ-PPh2)M(CO) 4 (M-Cr.Mo, W) complel catalysts catalyzing CO2 hydrogenation are reported.The catalysts exhibited high catalytic activity and selectivity toward oxygenates
A facile and user friendly technique to immobilize the late-transition metal complexes on spherical MgCl2/SiO2/THF support has been developed. The spherical MgCl2/SiO2/THF-supported late-transition metal catalysts 2,6...A facile and user friendly technique to immobilize the late-transition metal complexes on spherical MgCl2/SiO2/THF support has been developed. The spherical MgCl2/SiO2/THF-supported late-transition metal catalysts 2,6-bis-[1-(2,6-dimethylphenylimino)ethyl]pyridine iron(II) dichloride(SC-A) and 1,4-bis(2,6-dimethylphenyl)- acenaphthene diimine nickel(II) dibromide(SC-B) for ethylene polymerization has been prepared by spray-drying technique using tetrahydrofuran suspension containing MgCl2, SiO2 and late-transition metal complexes. The catalysts were characterized by BET, XRD, SEM and the polymers were analyzed using GPC, DSC and 13C-NMR. The test results show that spray-drying is a very effective method for immobilizing late-transition metal catalysts for ethylene polymerization. Among six kinds of cocatalysts for olefin polymerization, TMA and TEA were confirmed to be more effective than other compounds for the ethylene polymerization system using the catalyst SC-A. For the case of the catalyst SC-B, DEAC showed the best performance as cocatalysts in ethylene polymerization. The replication of the catalyst morphology was found in the resultant polyethylene.展开更多
Highly active solid superacid catalysts for n-butane isomerization, SZ/A1_2O_3-P, were prepared by supporting SO-(4-2)/ZrO2, (SZ) on y-A1_2O_3 carrier using a precipitation method. The activities of some catalysts wer...Highly active solid superacid catalysts for n-butane isomerization, SZ/A1_2O_3-P, were prepared by supporting SO-(4-2)/ZrO2, (SZ) on y-A1_2O_3 carrier using a precipitation method. The activities of some catalysts were enhanced significantly j The activity of the most active sample. 60%SZ/Al_2O3-P, was even about 2 times more active than that of the SZ catalyst.展开更多
In the preparation of catalyst for propylene polymerization, the Mg(OEt) 2 support was activated with ethanol/CO 2 system followed by solidification, and treated with TiCl 4 in the presence of ethylbenzoate as an inte...In the preparation of catalyst for propylene polymerization, the Mg(OEt) 2 support was activated with ethanol/CO 2 system followed by solidification, and treated with TiCl 4 in the presence of ethylbenzoate as an internal donor(ID). The chemical compositions of the activated support and the prepared catalyst were examined in detail. During the dissolution of Mg(OEt) 2 support in ethanol medium with CO 2 bubbling, the structure of support changed to magnesium hydrocarbyl carbonate, (CH 3CH 2O) 2- x Mg(O (C O) OCH 2CH 3) x ( x = 1,2). The content of carbonated CO 2 in the activated support was dependent on the heat treatment in the solidification of support. In the preparation procedure of polymerization catalyst, the activated support was treated with TiCl 4 so that the structure of support was converted to MgCl 2 with the incorporation of ID. The polymerization behavior of the pre-pared catalyst was also studied in the presence of phenyltriethoxysilane as an external donor.展开更多
The deposition of NH4 HSO4 and the poisoning effect of SO2 on SCR catalyst are the main obstacles that restrict the industrial application of CeO2-doped SCR catalysts.In this work,deposited NH4 HSO4 decomposition beha...The deposition of NH4 HSO4 and the poisoning effect of SO2 on SCR catalyst are the main obstacles that restrict the industrial application of CeO2-doped SCR catalysts.In this work,deposited NH4 HSO4 decomposition behavior and SO2 poisoning over V2 O5-MoO3/TiO2 catalysts modified with CeO2 and SiO2 were investigated.By the means of characterization analysis,it was found that the addition of SiO2 into VMo/Ti-Ce had an impact on the interaction existed between catalyst surface atoms and NH4 HSO4.Temperatureprogrammed methods and in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)experiments indicated that the doping of SiO2 promoted the decomposition of deposited NH4 HSO4 on VMo/Ti-Ce catalyst surface by reducing the thermal stability of NH4 HSO4 and enhancing the NH4 HSO4 reactivity with NO in low temperature.And this improvement may be the reason for the better catalytic activity than VMo/Ti-Ce in the case of NH4 HSO4 deposition.Accompanied with cerium sulfate species generated over catalyst surface,the conversion of SO2 to SO3 was inhibited in SiCe mixed catalyst.The addition of SiO2 could promote the decomposition of cerium sulfate,which may be a potential strategy to enhance the resistance of SO2 poisoning over CeO2-modifed catalysts.展开更多
Polyethylene (PE) grafting 4-vinylpyridine copolymers has been produced as powders of different rushes by theirradiation method. After treatment with methylaluminoxane (MAO), the copolymers were used as supports for C...Polyethylene (PE) grafting 4-vinylpyridine copolymers has been produced as powders of different rushes by theirradiation method. After treatment with methylaluminoxane (MAO), the copolymers were used as supports for Cp_2ZrCl_2catalyst Results of X-ray photoelectron spectroscopy, Fourier transforms infrared spectroscopy, ultraviolet spectroscopy andscanning electron microscope measurements show that the catalytic sites have been linked through MAO on the PE-graft-4-vinylpyridine (PEVP). The percentages of grafting 4-vinylpyridine and supported Cp_2ZrCl_2 depend on the size ofpolyethylene powder. The smaller the polyethylene powder, the more percent of 4-vinylpyridine groups and Cp_2ZrCl_2 existon the polyethylene chains, and the PEVP-supported catalyst has a relatively high activity for ethylene polymerization.展开更多
In this work,the influence of CO2 on the structural variation and catalytic performance of Na2WO4/Mn/Si O2 for oxidative coupling of methane to ethylene was investigated. The catalyst was prepared by impregnation meth...In this work,the influence of CO2 on the structural variation and catalytic performance of Na2WO4/Mn/Si O2 for oxidative coupling of methane to ethylene was investigated. The catalyst was prepared by impregnation method and characterized by XRD,Raman and XPS techniques. Appropriate amount of CO2 in the reactant gases enhanced the formation of surface tetrahedral Na2WO4 species and promoted the migration of O in MOx,Na,W from the catalyst bulk to surface,which were favorable for oxidative coupling of methane. When the molar ratio of CH4/O2/CO2 was 3/1/2,enriched surface tetrahedral Na2WO4 species and high surface concentration of O in MOx,Na,W were detected,and then high CH4 conversion of 33.1% and high C2H4 selectivity of 56.2% were obtained. With further increase of CO2 in the reagent gases,the content of active surface tetrahedral Na2WO4 species and surface concentration of O in MOx,Na,W decreased,while that of inactive species（Mn WO4 and Mn2O3） increased dramatically,leading to low CH4 conversion and low C2H4 selectivity. It could be speculated that Na2WO4 crystal was transformed into Mn WO4 crystal with excessive CO2 added under the reaction conditions. Pretreatment of Na2WO4/Mn/Si O2 catalyst by moderate amount of CO2 before OCM also promoted the formation of Na2WO4 species.展开更多
Pt-CeO2-ZrO2/MgO （Pt-CZ/MgO） catalysts with 0.8 wt% Pt, 3.0 wt% CeO2 and 3.0 wt% ZrO2 were prepared by wet impregnation method. Support MgO was obtained using ion exchange resin method or using commercial MgO. XRD, ...Pt-CeO2-ZrO2/MgO （Pt-CZ/MgO） catalysts with 0.8 wt% Pt, 3.0 wt% CeO2 and 3.0 wt% ZrO2 were prepared by wet impregnation method. Support MgO was obtained using ion exchange resin method or using commercial MgO. XRD, BET, SEM, TEM, DTA-TG and CO2-TPD were used to characterize the catalysts. CH4-CO2 reforming to synthesis gas （syngas） was performed to test the catalytic behavior of the catalysts. The catalyst Pt-CZ/MgO-IE（D） prepared using ion exchange resin exhibits more regular structure, smaller and more unique particle sizes, and stronger basicity than the catalyst Pt-CZ/MgO prepared from commercial MgO. At 1073 K and atmospheric pressure, Pt-CZ/MgO-IE（D） catalyst has a higher activity and greater stability than Pt-CZ/MgO catalyst for CH4-CO2 reforming reaction at high gas hourly space velocity of 36000 mL/（g.h） with a stoichiometric feed of CH4 and C02. Activity measurement and characterization results demonstrate that modification of the support using ion exchange resin method can promote the surface structural property and stability, therefore enhancing the activity and stability for CH4-CO2 reforming reaction.展开更多
The Fischer–Tropsch to olefins（FTO） process is a method for the direct conversion of synthesis gas to lower C–Colefins. Carbon-supported iron carbide nanoparticles are attractive catalysts for this reaction.The ca...The Fischer–Tropsch to olefins（FTO） process is a method for the direct conversion of synthesis gas to lower C–Colefins. Carbon-supported iron carbide nanoparticles are attractive catalysts for this reaction.The catalytic activity can be improved and undesired formation of alkanes can be suppressed by the addition of sodium and sulfur as promoters but the influence of their content and ratio remains poorly understood and the promoted catalysts often suffer from rapid deactivation due to particle growth. A series of carbon black-supported iron catalysts with similar iron content and nominal sodium/sulfur loadings of 1–30/0.5–5 wt% with respect to iron are prepared and characterized under FTO conditions at 1and 10 bar syngas pressure to illuminate the influence of the promoter level on the catalytic properties.Iron particles and promoters undergo significant reorganization during FTO operation under industrially relevant conditions. Low sodium content（1–3 wt%） leads to a delay in iron carbide formation. Sodium contents of 15–30 wt% lead to rapid loss of catalytic activity due to the covering of the iron surface with promoters during particle growth under FTO operation. Higher activity and slower loss of activity are observed at low promoter contents（1–3 wt% sodium and 0.5–1 wt% sulfur） but a minimum amount of alkali is required to effectively suppress methane and C–Cparaffin formation. A reference catalyst support（carbide-derived carbon aerogel） shows that the optimum promoter level depends on iron particle size and support pore structure.展开更多
Hydroxylation of inert benzene through the activation of the C_(sp2)-H bond is a representative reaction about the transformation of C-H bonds to C-O bonds,which has far-reaching guiding significance but remains a cha...Hydroxylation of inert benzene through the activation of the C_(sp2)-H bond is a representative reaction about the transformation of C-H bonds to C-O bonds,which has far-reaching guiding significance but remains a challenging scientific problem.To overcome this problem,a series of VOx-Ga_(2)O_(3)/SiO_(2)-Al_(2)O_(3)were prepared to achieve an efficient and economical hydroxylation path of benzene to phenol.The results showed that the phenol yield was 72.89%(selectivity>98.1%)under the optimum conditions.The reason is that the C-H bond in the benzene ring is activated by heterolysis over a VOx-Ga_(2)O_(3)/SiO_(2)-Al_(2)O_(3)catalyst.Meanwhile,the introduction of aluminum(Al)and gallium(Ga)made a qualitative change in the catalyst,enhancing the electron motion and spin motion of vanadium species,resulting in the increase of V4^(+)/V5^(+)ratio.In addition,the catalyst can provide an optimal acidic environment and a threedimensional cross-linked surface structure that facilitates product diffusion.展开更多
A novel Ni-Co/SiO2 catalyst which exhibits high activity and excellent anti-carbon deposition property for CO2 reforming of CH4 to synthesis gas is developed.
基金supported by the Natural Science Foundation of Shanxi Province(202203021221155)the Foundation of National Key Laboratory of High Efficiency and Low Carbon Utilization of Coal(J23-24-902)。
文摘With ongoing global warming and increasing energy demands,the CH_(4)-CO_(2)reforming reaction(dry reforming of methane,DRM)has garnered significant attention as a promising carbon capture and utilization technology.Nickel-based catalysts are renowned for their outstanding activity and selectivity in this process.The impact of metal-support interaction(MSI),on Ni-based catalyst performance has been extensively researched and debated recently.This paper reviews the recent research progress of MSI on Ni-based catalysts and their characterization and modulation strategies in catalytic reactions.From the perspective of MSI,the effects of different carriers(metal oxides,carbon materials and molecular sieves,etc.)are introduced on the dispersion and surface structure of Ni active metal particles,and the effect of MSI on the activity and stability of DRM reactions on Ni-based catalysts is discussed in detail.Future research should focus on better understanding and controlling MSI to improve the performance and durability of nickel-based catalysts in CH_(4)-CO_(2)reforming,advancing cleaner energy technologies.
基金The Executive Programme for Cooperation between Italy and India (Prot.No.MAE01054762017)。
文摘Nickel and nickel-ceria catalysts supported on high surface area silica, with 6 wt% Ni and 20 wt% CeO2 were prepared by microwave assisted(co) precipitation method. The catalysts were investigated by XRD,TPR and XPS analyses and they were tested in partial oxidation of methane(CPO). The catalytic reaction was carried out at atmospheric pressure in a temperature range of 400–800℃ with a feed gas mixture containing methane and oxygen in a molecular ratio CH4/O2=2. The Ni catalyst exhibited 60% methane conversion with 60% selectivity to CO already at 500℃. On the contrary, the Ni–Ce catalyst was inert to CPO up to 700℃. Moreover, the former catalyst reproduced its activity at the descending temperatures maintaining a good stability at 600℃, over a reaction time of 80 h, whereas the latter one completely deactivated. Test of CH4 temperature programmed surface reaction(CH4-TPSR) revealed a higher methane activation temperature(> 100℃) for the Ni–Ce catalyst as compared to the Ni one. Noticeable improvement of the ceria containing catalyst occurred when the reaction test started at a temperature higher than the methane decomposition temperature. In this case, the sample achieved the same catalytic behavior of the Ni catalyst. As confirmed by XPS analyses, the distinct electronic state of the supported nickel was responsible for the differences in catalytic behavior.
基金supported by the National Natural Science Foundation of China (Grant No.U1162114)the Science Foundation of Tianjin University of Science & Technology (20090420)
文摘A facile and user friendly technique to immobilize the late-transition metal complexes on spherical MgCl2/SiO2/THF support has been developed. The spherical MgCl2/SiO2/THF-supported late-transition metal catalysts 2,6-bis-[1-(2,6-dimethylphenylimino)ethyl]pyridine iron(II) dichloride(SC-A) and 1,4-bis(2,6-dimethylphenyl)- acenaphthene diimine nickel(II) dibromide(SC-B) for ethylene polymerization has been prepared by spray-drying technique using tetrahydrofuran suspension containing MgCl2, SiO2 and late-transition metal complexes. The catalysts were characterized by BET, XRD, SEM and the polymers were analyzed using GPC, DSC and 13C-NMR. The test results show that spray-drying is a very effective method for immobilizing late-transition metal catalysts for ethylene polymerization. Among six kinds of cocatalysts for olefin polymerization, TMA and TEA were confirmed to be more effective than other compounds for the ethylene polymerization system using the catalyst SC-A. For the case of the catalyst SC-B, DEAC showed the best performance as cocatalysts in ethylene polymerization. The replication of the catalyst morphology was found in the resultant polyethylene.
文摘Highly active solid superacid catalysts for n-butane isomerization, SZ/A1_2O_3-P, were prepared by supporting SO-(4-2)/ZrO2, (SZ) on y-A1_2O_3 carrier using a precipitation method. The activities of some catalysts were enhanced significantly j The activity of the most active sample. 60%SZ/Al_2O3-P, was even about 2 times more active than that of the SZ catalyst.
文摘In the preparation of catalyst for propylene polymerization, the Mg(OEt) 2 support was activated with ethanol/CO 2 system followed by solidification, and treated with TiCl 4 in the presence of ethylbenzoate as an internal donor(ID). The chemical compositions of the activated support and the prepared catalyst were examined in detail. During the dissolution of Mg(OEt) 2 support in ethanol medium with CO 2 bubbling, the structure of support changed to magnesium hydrocarbyl carbonate, (CH 3CH 2O) 2- x Mg(O (C O) OCH 2CH 3) x ( x = 1,2). The content of carbonated CO 2 in the activated support was dependent on the heat treatment in the solidification of support. In the preparation procedure of polymerization catalyst, the activated support was treated with TiCl 4 so that the structure of support was converted to MgCl 2 with the incorporation of ID. The polymerization behavior of the pre-pared catalyst was also studied in the presence of phenyltriethoxysilane as an external donor.
基金supported by the National Natural Science Foundation of China(No.51576039)
文摘The deposition of NH4 HSO4 and the poisoning effect of SO2 on SCR catalyst are the main obstacles that restrict the industrial application of CeO2-doped SCR catalysts.In this work,deposited NH4 HSO4 decomposition behavior and SO2 poisoning over V2 O5-MoO3/TiO2 catalysts modified with CeO2 and SiO2 were investigated.By the means of characterization analysis,it was found that the addition of SiO2 into VMo/Ti-Ce had an impact on the interaction existed between catalyst surface atoms and NH4 HSO4.Temperatureprogrammed methods and in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)experiments indicated that the doping of SiO2 promoted the decomposition of deposited NH4 HSO4 on VMo/Ti-Ce catalyst surface by reducing the thermal stability of NH4 HSO4 and enhancing the NH4 HSO4 reactivity with NO in low temperature.And this improvement may be the reason for the better catalytic activity than VMo/Ti-Ce in the case of NH4 HSO4 deposition.Accompanied with cerium sulfate species generated over catalyst surface,the conversion of SO2 to SO3 was inhibited in SiCe mixed catalyst.The addition of SiO2 could promote the decomposition of cerium sulfate,which may be a potential strategy to enhance the resistance of SO2 poisoning over CeO2-modifed catalysts.
基金National Natural Science Foundation of China (No. 20272062)
文摘Polyethylene (PE) grafting 4-vinylpyridine copolymers has been produced as powders of different rushes by theirradiation method. After treatment with methylaluminoxane (MAO), the copolymers were used as supports for Cp_2ZrCl_2catalyst Results of X-ray photoelectron spectroscopy, Fourier transforms infrared spectroscopy, ultraviolet spectroscopy andscanning electron microscope measurements show that the catalytic sites have been linked through MAO on the PE-graft-4-vinylpyridine (PEVP). The percentages of grafting 4-vinylpyridine and supported Cp_2ZrCl_2 depend on the size ofpolyethylene powder. The smaller the polyethylene powder, the more percent of 4-vinylpyridine groups and Cp_2ZrCl_2 existon the polyethylene chains, and the PEVP-supported catalyst has a relatively high activity for ethylene polymerization.
基金support from the Ministry of Science and Technology (Nos.2012BAC20B10)the National Natural Science Foundation of China (Nos. 21321061 and 20976109)
文摘In this work,the influence of CO2 on the structural variation and catalytic performance of Na2WO4/Mn/Si O2 for oxidative coupling of methane to ethylene was investigated. The catalyst was prepared by impregnation method and characterized by XRD,Raman and XPS techniques. Appropriate amount of CO2 in the reactant gases enhanced the formation of surface tetrahedral Na2WO4 species and promoted the migration of O in MOx,Na,W from the catalyst bulk to surface,which were favorable for oxidative coupling of methane. When the molar ratio of CH4/O2/CO2 was 3/1/2,enriched surface tetrahedral Na2WO4 species and high surface concentration of O in MOx,Na,W were detected,and then high CH4 conversion of 33.1% and high C2H4 selectivity of 56.2% were obtained. With further increase of CO2 in the reagent gases,the content of active surface tetrahedral Na2WO4 species and surface concentration of O in MOx,Na,W decreased,while that of inactive species（Mn WO4 and Mn2O3） increased dramatically,leading to low CH4 conversion and low C2H4 selectivity. It could be speculated that Na2WO4 crystal was transformed into Mn WO4 crystal with excessive CO2 added under the reaction conditions. Pretreatment of Na2WO4/Mn/Si O2 catalyst by moderate amount of CO2 before OCM also promoted the formation of Na2WO4 species.
基金supported by the National Natural Science Foundation of China (No. 20873013)
文摘Pt-CeO2-ZrO2/MgO （Pt-CZ/MgO） catalysts with 0.8 wt% Pt, 3.0 wt% CeO2 and 3.0 wt% ZrO2 were prepared by wet impregnation method. Support MgO was obtained using ion exchange resin method or using commercial MgO. XRD, BET, SEM, TEM, DTA-TG and CO2-TPD were used to characterize the catalysts. CH4-CO2 reforming to synthesis gas （syngas） was performed to test the catalytic behavior of the catalysts. The catalyst Pt-CZ/MgO-IE（D） prepared using ion exchange resin exhibits more regular structure, smaller and more unique particle sizes, and stronger basicity than the catalyst Pt-CZ/MgO prepared from commercial MgO. At 1073 K and atmospheric pressure, Pt-CZ/MgO-IE（D） catalyst has a higher activity and greater stability than Pt-CZ/MgO catalyst for CH4-CO2 reforming reaction at high gas hourly space velocity of 36000 mL/（g.h） with a stoichiometric feed of CH4 and C02. Activity measurement and characterization results demonstrate that modification of the support using ion exchange resin method can promote the surface structural property and stability, therefore enhancing the activity and stability for CH4-CO2 reforming reaction.
基金supported by a Post Doc grant of the German Academic Exchange Service(Deutscher Akademischer Austauschdienst,DAAD grant no.91552012)by the European Research Council(EU FP7 ERC advanced grant no.338846)
文摘The Fischer–Tropsch to olefins（FTO） process is a method for the direct conversion of synthesis gas to lower C–Colefins. Carbon-supported iron carbide nanoparticles are attractive catalysts for this reaction.The catalytic activity can be improved and undesired formation of alkanes can be suppressed by the addition of sodium and sulfur as promoters but the influence of their content and ratio remains poorly understood and the promoted catalysts often suffer from rapid deactivation due to particle growth. A series of carbon black-supported iron catalysts with similar iron content and nominal sodium/sulfur loadings of 1–30/0.5–5 wt% with respect to iron are prepared and characterized under FTO conditions at 1and 10 bar syngas pressure to illuminate the influence of the promoter level on the catalytic properties.Iron particles and promoters undergo significant reorganization during FTO operation under industrially relevant conditions. Low sodium content（1–3 wt%） leads to a delay in iron carbide formation. Sodium contents of 15–30 wt% lead to rapid loss of catalytic activity due to the covering of the iron surface with promoters during particle growth under FTO operation. Higher activity and slower loss of activity are observed at low promoter contents（1–3 wt% sodium and 0.5–1 wt% sulfur） but a minimum amount of alkali is required to effectively suppress methane and C–Cparaffin formation. A reference catalyst support（carbide-derived carbon aerogel） shows that the optimum promoter level depends on iron particle size and support pore structure.
基金the Support Program for Hongliu Young Teachers of Lanzhou University of Technology(02/062214)Young Talent Innovation Project of Lanzhou(2023-QN-103)Major science and technology projects of Gansu Province(22ZD6GA013).
文摘Hydroxylation of inert benzene through the activation of the C_(sp2)-H bond is a representative reaction about the transformation of C-H bonds to C-O bonds,which has far-reaching guiding significance but remains a challenging scientific problem.To overcome this problem,a series of VOx-Ga_(2)O_(3)/SiO_(2)-Al_(2)O_(3)were prepared to achieve an efficient and economical hydroxylation path of benzene to phenol.The results showed that the phenol yield was 72.89%(selectivity>98.1%)under the optimum conditions.The reason is that the C-H bond in the benzene ring is activated by heterolysis over a VOx-Ga_(2)O_(3)/SiO_(2)-Al_(2)O_(3)catalyst.Meanwhile,the introduction of aluminum(Al)and gallium(Ga)made a qualitative change in the catalyst,enhancing the electron motion and spin motion of vanadium species,resulting in the increase of V4^(+)/V5^(+)ratio.In addition,the catalyst can provide an optimal acidic environment and a threedimensional cross-linked surface structure that facilitates product diffusion.
基金the Zhejiang Provincial Science Foundation of China and by the Education Commission of Zhejiang Province.
文摘A novel Ni-Co/SiO2 catalyst which exhibits high activity and excellent anti-carbon deposition property for CO2 reforming of CH4 to synthesis gas is developed.
