Among challenges implicit in the transition to the post-fossil fuel energetic model,the finite amount of resources available for the technological implementation of CO_(2) revalorizing processes arises as a central is...Among challenges implicit in the transition to the post-fossil fuel energetic model,the finite amount of resources available for the technological implementation of CO_(2) revalorizing processes arises as a central issue.The development of fully renewable catalytic systems with easier metal recovery strategies would promote the viability and sustainability of synthetic natural gas production circular routes.Taking Ni and NiFe catalysts supported over g-Al_(2)O_(3) oxide as reference materials,this work evaluates the potentiality of Ni and NiFe supported biochar catalysts for CO_(2) methanation.The development of competitive biochar catalysts was found dependent on the creation of basic sites on the catalyst surface.Displaying lower Turn Over Frequencies than Ni/Al catalyst,the absence of basic sites achieved over Ni/C catalyst was related to the depleted catalyst performances.For NiFe catalysts,analogous Ni_(5)Fe_(1) alloys were constituted over both alumina and biochar supports.The highest specific activity of the catalyst series,exhibited by the NiFe/C catalyst,was related to the development of surface basic sites along with weaker NiFe-C interactions,which resulted in increased Ni0:NiO surface populations under reaction conditions.In summary,the present work establishes biochar supports as a competitive material to consider within the future low-carbon energetic panorama.展开更多
Composite supports CeO2-ZrO2-Al2O3(CZA) and CeO2-ZrO2-Al2O3-La2O3(CZALa) were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and N...Composite supports CeO2-ZrO2-Al2O3(CZA) and CeO2-ZrO2-Al2O3-La2O3(CZALa) were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and NOx in the mixture gas simulated the exhaust from natural gas vehicles (NGVs) operated under stoichiometric condition was investigated. The effect of La2O3 on the physicochemical properties of supports and catalysts was characterized by various techniques. The characterizations with X-ray diffraction (XRD) and Raman spectroscopy revealed that the doping of La2O3 restrained effectively the sintering of crystallite particles, maintained the crystallite particles in nanoscale and stabilized the crystal phase after calcination at 1000 ℃. The results of N2-adsorption, H2-temperatnre-programmed reduction (H2-TPR) and oxygen storage capacity (OSC) measurements indicated that La2O3 improved the textural properties, reducibility and OSC of composite supports. Activity testing results showed that the catalysts exhibit excellent activities for the simultaneous removal of methane, CO and NOx in the simulated exhaust gas. The catalysts supported on CZALa showed remarkable thermal stability and catalytic activity for the three pollutants, especially for NOx. The prepared palladium catalysts have high ability to remove NOx, CH4 and CO, and they can be used as excellent catalysts for the purification of exhaust from NGVs operated under stoichiometric condition. The catalysts reported in this work also have significant potential in industrial application because of their high performance and low cost.展开更多
Pd-based catalysts modified by cobalt were prepared by co-impregnation and sequential impregnation methods,and characterized by X-ray powder diffraction (XRD),N2 adsorption/desorption (Brunauer-Emmet-Teller method...Pd-based catalysts modified by cobalt were prepared by co-impregnation and sequential impregnation methods,and characterized by X-ray powder diffraction (XRD),N2 adsorption/desorption (Brunauer-Emmet-Teller method),CO-chemisorption and X-ray photoelectron spectroscopy (XPS).The activity of Pd catalysts was tested in the simulated exhaust gas from lean-burn natural gas vehicles.The effect of Co on the performance of water poisoning resistance for Pd catalysts was estimated in the simulated exhaust gas with and without the presence of water vapor.It was found that the effect of Co significantly depended on the preparation process.PdCo/La-Al2O3 catalyst prepared by co-impregnation exhibited better water-resistant performance.The results of XPS indicated that both CoAl2O4 and Co3O4 were present in the Pd catalysts modified by Co.For the catalyst prepared by sequential impregnation method,the ratio of CoAl2O4/Co3O4 was higher than that of the catalyst prepared by co-impregnation method.It could be concluded that Co3O4 played an important role in improving water-resistant performance.展开更多
A three-way catalyst comprised novel oxygen storage components for emission control in natural gas powered engines was prepared. The addition of novel oxygen storage components to the Pd/γ-Al2O3 catalysts resulted ...A three-way catalyst comprised novel oxygen storage components for emission control in natural gas powered engines was prepared. The addition of novel oxygen storage components to the Pd/γ-Al2O3 catalysts resulted in improved activities of the fresh and aged catalyst by lowering the light-off temperature for methane in natural gas engines exhaust.展开更多
An efficient and greener synthesis of a series of dihydropyrimidinone (DHPMs) derivatives were accomplished via three-component one-pot cyclocondensation between substituted aryl aldehydes, diketone/ke- toester and ur...An efficient and greener synthesis of a series of dihydropyrimidinone (DHPMs) derivatives were accomplished via three-component one-pot cyclocondensation between substituted aryl aldehydes, diketone/ke- toester and urea. This solvent free approach is totally nonpolluting having several advantages such as shorter reaction time, mild reaction conditions, simple workup and reduced environmental impact.展开更多
The DS-1 catalyst for energy-saving natural gas steam reforming was preparedby using potash as a carbon-resistant additive and adding rare earth oxide. The catalystdemonstrated good reducibility, carbon resistance, ac...The DS-1 catalyst for energy-saving natural gas steam reforming was preparedby using potash as a carbon-resistant additive and adding rare earth oxide. The catalystdemonstrated good reducibility, carbon resistance, activity and stability in aging tests and 500 hstability tests at low water/carbon ratios.展开更多
In order to develop high-efficiency and low-cost catalyst for the slurry-phase hydrocracking of vacuum residue(VR),the catalyst supported on natural rectorite was prepared,and the effect of calcination modification of...In order to develop high-efficiency and low-cost catalyst for the slurry-phase hydrocracking of vacuum residue(VR),the catalyst supported on natural rectorite was prepared,and the effect of calcination modification of rectorite on the catalyst properties and performance was investigated.The support of rectorite and catalyst were characterized by XRD,FTIR,Py-FTIR,H_(2)-TPR and XPS to examine their structures and properties.The comparative reaction results show that VR conversions for the catalysts supported on calcined rectorite were similar with that on raw rectorite,possibly due to the VR cracking reaction controlled by the thermal cracking following free radical mechanism because of few acid sites observed on the catalysts surface.However,the yields of naphtha and middle distillates for the various catalysts were obviously different,and increased following as Rec-Mo(40.4 wt%)展开更多
Kapok seed oil is an environmentally friendly biodiesel feedstock.The problem of the best catalyst for transester-ification of Kapok seed oil still continues today.The research developed a base-heterogeneous catalyst ...Kapok seed oil is an environmentally friendly biodiesel feedstock.The problem of the best catalyst for transester-ification of Kapok seed oil still continues today.The research developed a base-heterogeneous catalyst with the effect of ultrasonic waves during transesterification.So,the study aims:(1)to determine the type of natural zeolite used,(2)to determine the characteristics of the synthesized CaO:BaO/ANZ catalyst,and(3)to determine the effectiveness of the CaO:BaO/ANZ catalyst in the biodiesel production process through sono-transeste rification of kapok seed oil.The research stages consisted of:(1)activation of natural zeolite and its characterization,(2)preparation of CaO:BaO/ANZ catalyst,(3)characterization of CaO:BaO/ANZ catalyst,(4)esterification and uti-lization of catalyst in the transesterification,(5)analysis of transesterified products.The results showed that the natural zeolite type from the southerm area of Malang is mordenite(MOR)type.Then,after the natural zeolite was impregnated,the obtained catalyst compositions were CaO:BaO-9:9/ANZ,CaO:BaO-14:9/ANZ,and CaO:BaO-4:11/ANZ with a surface area of 129.7;124.6;128.5 m^(2)/g,and acidity of 1.037;0.254;and 0.685 mmol/g,respectively.The best catalyst for transesterification of kapok seed oil was CaO:BaO-9:9/ANZ,which resulted in a biodiesel yield of 73.6%with a density of 889.6 kg/m^(3) and kinematic viscosity of 2.987 cSt.The characteristics of the produced biodiesel meet requirement of SNI 7182:2015.展开更多
We first obtained by impregnating the zeolite with salts U, W and V and examined the X-ray uranium catalyst SAPO-U, W, V based on natural zeolite Chankanayskogoe deposits for the oxidation of SO2 to SO3.
Decreasing supplies of high quality crude oil and increasing demand for high quality distillates have motivated the interest in converting natural gas to liquid fuels, especially with the present boom in natural gas p...Decreasing supplies of high quality crude oil and increasing demand for high quality distillates have motivated the interest in converting natural gas to liquid fuels, especially with the present boom in natural gas proven reserves. Nevertheless, one major issue is the curtailment of costs incurred in producing synthesis gas from natural gas, which account for approximately 60% of the costs used in producing liquid fuels. While there are three main routes to convert natural gas to syngas: steam reforming (SMR), partial Oxidation (POX) and auto-thermal reforming (ATR). Significant new developments and improvements in these technologies, established innovative processes to minimize greenhouse gases emission, minimize energy consumption, enhance syngas processes, adjust the desired H<sub>2</sub>/CO ratio and change the baseline economics. This article reviews the state of the art for the reforming of natural gas to synthesis gas taking into consideration all the new innovations in both processes and catalysis.展开更多
A series of alumina supported cobalt oxide based catalysts doped with noble metals such as ruthenium and platinum were prepared by wet impregnation method.The variables studied were difference ratio and calcination te...A series of alumina supported cobalt oxide based catalysts doped with noble metals such as ruthenium and platinum were prepared by wet impregnation method.The variables studied were difference ratio and calcination temperatures.Pt/Co(10∶90)/Al2O3 catalyst calcined at 700 ℃ was found to be the best catalyst which able to convert 70.10% of CO2 into methane with 47% of CH4 formation at maximum temperature studied of 400 ℃.X-ray diffraction analysis showed that this catalyst possessed the active site Co3O4 in face-centered cubic and PtO2 in the orthorhombic phase with Al2O3 existed in the cubic phase.According to the FESEM micrographs,both fresh and spent Pt/Co(10∶90)/Al2O3 catalysts displayed small particle size with undefined shape.Nitrogen Adsorption analysis showed that 5.50% reduction of the total surface area for the spent Pt/Co(10∶90)/Al2O3 catalyst.Meanwhile,Energy Dispersive X-ray analysis(EDX) indicated that Co and Pt were reduced by 0.74% and 0.14% respectively on the spent Pt/Co(10∶90)/Al2O3catalyst.Characterization using FT-IR and TGA-DTA analysis revealed the existence of residual nitrate and hydroxyl compounds on the Pt/Co(10∶90)/Al2O3 catalyst.展开更多
The correlation between phase structures and surface acidity of Al2O3 supports calcined at different temperatures and the catalytic performance of Ni/Al2O3 catalysts in the production of synthetic natural gas(SNG) via...The correlation between phase structures and surface acidity of Al2O3 supports calcined at different temperatures and the catalytic performance of Ni/Al2O3 catalysts in the production of synthetic natural gas(SNG) via CO methanation was systematically investigated. A series of 10 wt% NiO/Al2O3 catalysts were prepared by the conventional impregnation method, and the phase structures and surface acidity of Al2O3 supports were adjusted by calcining the commercial γ-Al2O3 at different temperatures(600–1200 C). CO methanation reaction was carried out in the temperature range of 300–600 C at different weight hourly space velocities(WHSV = 30000 and 120000 mL·g-1h-1) and pressures(0.1 and 3.0 MPa). It was found that high calcination temperature not only led to the growth in Ni particle size, but also weakened the interaction between Ni nanoparticles and Al2O3 supports due to the rapid decrease of the specific surface area and acidity of Al2O3 supports. Interestingly, Ni catalysts supported on Al2O3 calcined at 1200 C(Ni/Al2O3-1200) exhibited the best catalytic activity for CO methanation under different reaction conditions. Lifetime reaction tests also indicated that Ni/Al2O3-1200 was the most active and stable catalyst compared with the other three catalysts, whose supports were calcined at lower temperatures(600, 800 and 1000 C). These findings would therefore be helpful to develop Ni/Al2O3 methanation catalyst for SNG production.展开更多
Nickel-based catalysts represent the most commonly used systems for CO methanation.We have successfully prepared a Ni catalyst system supported on two-dimensional plasma-treated vermiculite(2D-PVMT)with a very low N...Nickel-based catalysts represent the most commonly used systems for CO methanation.We have successfully prepared a Ni catalyst system supported on two-dimensional plasma-treated vermiculite(2D-PVMT)with a very low Ni loading(0.5 wt%).The catalyst precursor was subjected to heat treatment via either conventional heat treatment(CHT)or the plasma irradiation method(PIM).The as-obtained CHT-Ni/PVMT and PIM-Ni/PVMT catalysts were characterized with scanning electron microscopy(SEM),energy dispersive X-ray(EDX),X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),inductively coupled plasma-atomic emission spectroscopy(ICP-AES)and high-angle annular dark field scanning transmission electron microscopy(HAADF-STEM).Additionally,CHT-NiO/PVMT and PIM-NiO/PVMT catalysts were characterized with hydrogen temperature programmed reduction(H2-TPR).Compared with CHT-Ni/PVMT,PIM-Ni/PVMT exhibited superior catalytic performance.The plasma treated catalyst PIM-Ni/PVMT achieved a CO conversion of93.5%and a turnover frequency(TOF)of 0.8537 s^-1,at a temperature of 450℃,a gas hourly space velocity of 6000 ml·g^-1·h^-1,a synthesis gas flow rate of 65 ml·min^-1,and a pressure of 1.5 MPa.Plasma irradiation may provide a successful strategy for the preparation of catalysts with very low metal loadings which exhibit excellent properties.展开更多
文摘Among challenges implicit in the transition to the post-fossil fuel energetic model,the finite amount of resources available for the technological implementation of CO_(2) revalorizing processes arises as a central issue.The development of fully renewable catalytic systems with easier metal recovery strategies would promote the viability and sustainability of synthetic natural gas production circular routes.Taking Ni and NiFe catalysts supported over g-Al_(2)O_(3) oxide as reference materials,this work evaluates the potentiality of Ni and NiFe supported biochar catalysts for CO_(2) methanation.The development of competitive biochar catalysts was found dependent on the creation of basic sites on the catalyst surface.Displaying lower Turn Over Frequencies than Ni/Al catalyst,the absence of basic sites achieved over Ni/C catalyst was related to the depleted catalyst performances.For NiFe catalysts,analogous Ni_(5)Fe_(1) alloys were constituted over both alumina and biochar supports.The highest specific activity of the catalyst series,exhibited by the NiFe/C catalyst,was related to the development of surface basic sites along with weaker NiFe-C interactions,which resulted in increased Ni0:NiO surface populations under reaction conditions.In summary,the present work establishes biochar supports as a competitive material to consider within the future low-carbon energetic panorama.
基金supported by the National Natural Science Foundation of China (No. 20773090, 20803049)the National High Technology Researchand Development Program of China (863 Program, No. 2006AA06Z347)the Specialized Research Fund for the Doctoral Program of Higher Education(20070610026)
文摘Composite supports CeO2-ZrO2-Al2O3(CZA) and CeO2-ZrO2-Al2O3-La2O3(CZALa) were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and NOx in the mixture gas simulated the exhaust from natural gas vehicles (NGVs) operated under stoichiometric condition was investigated. The effect of La2O3 on the physicochemical properties of supports and catalysts was characterized by various techniques. The characterizations with X-ray diffraction (XRD) and Raman spectroscopy revealed that the doping of La2O3 restrained effectively the sintering of crystallite particles, maintained the crystallite particles in nanoscale and stabilized the crystal phase after calcination at 1000 ℃. The results of N2-adsorption, H2-temperatnre-programmed reduction (H2-TPR) and oxygen storage capacity (OSC) measurements indicated that La2O3 improved the textural properties, reducibility and OSC of composite supports. Activity testing results showed that the catalysts exhibit excellent activities for the simultaneous removal of methane, CO and NOx in the simulated exhaust gas. The catalysts supported on CZALa showed remarkable thermal stability and catalytic activity for the three pollutants, especially for NOx. The prepared palladium catalysts have high ability to remove NOx, CH4 and CO, and they can be used as excellent catalysts for the purification of exhaust from NGVs operated under stoichiometric condition. The catalysts reported in this work also have significant potential in industrial application because of their high performance and low cost.
基金supported by the National Natural Science Foundation of China (20773090)the Ph.D.Programs Foundation of Ministry of Education of China (200806100009)
文摘Pd-based catalysts modified by cobalt were prepared by co-impregnation and sequential impregnation methods,and characterized by X-ray powder diffraction (XRD),N2 adsorption/desorption (Brunauer-Emmet-Teller method),CO-chemisorption and X-ray photoelectron spectroscopy (XPS).The activity of Pd catalysts was tested in the simulated exhaust gas from lean-burn natural gas vehicles.The effect of Co on the performance of water poisoning resistance for Pd catalysts was estimated in the simulated exhaust gas with and without the presence of water vapor.It was found that the effect of Co significantly depended on the preparation process.PdCo/La-Al2O3 catalyst prepared by co-impregnation exhibited better water-resistant performance.The results of XPS indicated that both CoAl2O4 and Co3O4 were present in the Pd catalysts modified by Co.For the catalyst prepared by sequential impregnation method,the ratio of CoAl2O4/Co3O4 was higher than that of the catalyst prepared by co-impregnation method.It could be concluded that Co3O4 played an important role in improving water-resistant performance.
基金the National Natural Science Foundation of China(No:20273043)the Ministry of Education of China for providing financial support for this project
文摘A three-way catalyst comprised novel oxygen storage components for emission control in natural gas powered engines was prepared. The addition of novel oxygen storage components to the Pd/γ-Al2O3 catalysts resulted in improved activities of the fresh and aged catalyst by lowering the light-off temperature for methane in natural gas engines exhaust.
文摘An efficient and greener synthesis of a series of dihydropyrimidinone (DHPMs) derivatives were accomplished via three-component one-pot cyclocondensation between substituted aryl aldehydes, diketone/ke- toester and urea. This solvent free approach is totally nonpolluting having several advantages such as shorter reaction time, mild reaction conditions, simple workup and reduced environmental impact.
文摘The DS-1 catalyst for energy-saving natural gas steam reforming was preparedby using potash as a carbon-resistant additive and adding rare earth oxide. The catalystdemonstrated good reducibility, carbon resistance, activity and stability in aging tests and 500 hstability tests at low water/carbon ratios.
基金National Key Research and Development program(2018YFA0209403)National Natural Science Foundation of China(Youth)program(21908027)for financing this research。
文摘In order to develop high-efficiency and low-cost catalyst for the slurry-phase hydrocracking of vacuum residue(VR),the catalyst supported on natural rectorite was prepared,and the effect of calcination modification of rectorite on the catalyst properties and performance was investigated.The support of rectorite and catalyst were characterized by XRD,FTIR,Py-FTIR,H_(2)-TPR and XPS to examine their structures and properties.The comparative reaction results show that VR conversions for the catalysts supported on calcined rectorite were similar with that on raw rectorite,possibly due to the VR cracking reaction controlled by the thermal cracking following free radical mechanism because of few acid sites observed on the catalysts surface.However,the yields of naphtha and middle distillates for the various catalysts were obviously different,and increased following as Rec-Mo(40.4 wt%)
基金The funding that has supported the work,namely:PNBP Universitas Negeri Malang to Dr.Sumari,M.Si.
文摘Kapok seed oil is an environmentally friendly biodiesel feedstock.The problem of the best catalyst for transester-ification of Kapok seed oil still continues today.The research developed a base-heterogeneous catalyst with the effect of ultrasonic waves during transesterification.So,the study aims:(1)to determine the type of natural zeolite used,(2)to determine the characteristics of the synthesized CaO:BaO/ANZ catalyst,and(3)to determine the effectiveness of the CaO:BaO/ANZ catalyst in the biodiesel production process through sono-transeste rification of kapok seed oil.The research stages consisted of:(1)activation of natural zeolite and its characterization,(2)preparation of CaO:BaO/ANZ catalyst,(3)characterization of CaO:BaO/ANZ catalyst,(4)esterification and uti-lization of catalyst in the transesterification,(5)analysis of transesterified products.The results showed that the natural zeolite type from the southerm area of Malang is mordenite(MOR)type.Then,after the natural zeolite was impregnated,the obtained catalyst compositions were CaO:BaO-9:9/ANZ,CaO:BaO-14:9/ANZ,and CaO:BaO-4:11/ANZ with a surface area of 129.7;124.6;128.5 m^(2)/g,and acidity of 1.037;0.254;and 0.685 mmol/g,respectively.The best catalyst for transesterification of kapok seed oil was CaO:BaO-9:9/ANZ,which resulted in a biodiesel yield of 73.6%with a density of 889.6 kg/m^(3) and kinematic viscosity of 2.987 cSt.The characteristics of the produced biodiesel meet requirement of SNI 7182:2015.
文摘We first obtained by impregnating the zeolite with salts U, W and V and examined the X-ray uranium catalyst SAPO-U, W, V based on natural zeolite Chankanayskogoe deposits for the oxidation of SO2 to SO3.
文摘Decreasing supplies of high quality crude oil and increasing demand for high quality distillates have motivated the interest in converting natural gas to liquid fuels, especially with the present boom in natural gas proven reserves. Nevertheless, one major issue is the curtailment of costs incurred in producing synthesis gas from natural gas, which account for approximately 60% of the costs used in producing liquid fuels. While there are three main routes to convert natural gas to syngas: steam reforming (SMR), partial Oxidation (POX) and auto-thermal reforming (ATR). Significant new developments and improvements in these technologies, established innovative processes to minimize greenhouse gases emission, minimize energy consumption, enhance syngas processes, adjust the desired H<sub>2</sub>/CO ratio and change the baseline economics. This article reviews the state of the art for the reforming of natural gas to synthesis gas taking into consideration all the new innovations in both processes and catalysis.
文摘A series of alumina supported cobalt oxide based catalysts doped with noble metals such as ruthenium and platinum were prepared by wet impregnation method.The variables studied were difference ratio and calcination temperatures.Pt/Co(10∶90)/Al2O3 catalyst calcined at 700 ℃ was found to be the best catalyst which able to convert 70.10% of CO2 into methane with 47% of CH4 formation at maximum temperature studied of 400 ℃.X-ray diffraction analysis showed that this catalyst possessed the active site Co3O4 in face-centered cubic and PtO2 in the orthorhombic phase with Al2O3 existed in the cubic phase.According to the FESEM micrographs,both fresh and spent Pt/Co(10∶90)/Al2O3 catalysts displayed small particle size with undefined shape.Nitrogen Adsorption analysis showed that 5.50% reduction of the total surface area for the spent Pt/Co(10∶90)/Al2O3 catalyst.Meanwhile,Energy Dispersive X-ray analysis(EDX) indicated that Co and Pt were reduced by 0.74% and 0.14% respectively on the spent Pt/Co(10∶90)/Al2O3catalyst.Characterization using FT-IR and TGA-DTA analysis revealed the existence of residual nitrate and hydroxyl compounds on the Pt/Co(10∶90)/Al2O3 catalyst.
基金supported by the Hundred Talents Program of the Chinese Academy of Sciences (CAS),State Key Laboratory of Multiphase Complex Systems of China (No.MPCS-2009-C-01)the National Key Technology R&D Program of China (No.2010BAC66B01)the Knowledge Innovation Program of the CAS (No.KGCX2-YW-396)
文摘The correlation between phase structures and surface acidity of Al2O3 supports calcined at different temperatures and the catalytic performance of Ni/Al2O3 catalysts in the production of synthetic natural gas(SNG) via CO methanation was systematically investigated. A series of 10 wt% NiO/Al2O3 catalysts were prepared by the conventional impregnation method, and the phase structures and surface acidity of Al2O3 supports were adjusted by calcining the commercial γ-Al2O3 at different temperatures(600–1200 C). CO methanation reaction was carried out in the temperature range of 300–600 C at different weight hourly space velocities(WHSV = 30000 and 120000 mL·g-1h-1) and pressures(0.1 and 3.0 MPa). It was found that high calcination temperature not only led to the growth in Ni particle size, but also weakened the interaction between Ni nanoparticles and Al2O3 supports due to the rapid decrease of the specific surface area and acidity of Al2O3 supports. Interestingly, Ni catalysts supported on Al2O3 calcined at 1200 C(Ni/Al2O3-1200) exhibited the best catalytic activity for CO methanation under different reaction conditions. Lifetime reaction tests also indicated that Ni/Al2O3-1200 was the most active and stable catalyst compared with the other three catalysts, whose supports were calcined at lower temperatures(600, 800 and 1000 C). These findings would therefore be helpful to develop Ni/Al2O3 methanation catalyst for SNG production.
基金Supported by the National Natural Science Foundation of China(U1203293,21163015)the Doctor Foundation of Bingtuan(2013BB010)+1 种基金Program of Science and Technology Innovation Team in Bingtuan(2015BD003)Program for Changjiang Scholars,Innovative Research Team in University(IRT_15R46)
文摘Nickel-based catalysts represent the most commonly used systems for CO methanation.We have successfully prepared a Ni catalyst system supported on two-dimensional plasma-treated vermiculite(2D-PVMT)with a very low Ni loading(0.5 wt%).The catalyst precursor was subjected to heat treatment via either conventional heat treatment(CHT)or the plasma irradiation method(PIM).The as-obtained CHT-Ni/PVMT and PIM-Ni/PVMT catalysts were characterized with scanning electron microscopy(SEM),energy dispersive X-ray(EDX),X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),inductively coupled plasma-atomic emission spectroscopy(ICP-AES)and high-angle annular dark field scanning transmission electron microscopy(HAADF-STEM).Additionally,CHT-NiO/PVMT and PIM-NiO/PVMT catalysts were characterized with hydrogen temperature programmed reduction(H2-TPR).Compared with CHT-Ni/PVMT,PIM-Ni/PVMT exhibited superior catalytic performance.The plasma treated catalyst PIM-Ni/PVMT achieved a CO conversion of93.5%and a turnover frequency(TOF)of 0.8537 s^-1,at a temperature of 450℃,a gas hourly space velocity of 6000 ml·g^-1·h^-1,a synthesis gas flow rate of 65 ml·min^-1,and a pressure of 1.5 MPa.Plasma irradiation may provide a successful strategy for the preparation of catalysts with very low metal loadings which exhibit excellent properties.