Bio-silica issued from diatom, a microalgae, is attracted increasing attention in material science thanks to its peculiar nanoarchitecture and related properties with versatile applications. The present work is a deep...Bio-silica issued from diatom, a microalgae, is attracted increasing attention in material science thanks to its peculiar nanoarchitecture and related properties with versatile applications. The present work is a deep analysis on morphological and chemical properties of bio-silica issued from fossil origin (diatomaceous earth) and living one (algal paste). An optimization in purification protocol was performed to obtain multiparous bio-silica from its raw media with keeping its original shape entirely. Multiple characterization methods as scanning electronic microscopy (SEM), infrared spectroscopy, x-ray diffraction (DRX), X-ray photoelectron spectroscopy (XPS), energy dispersive X-ray spectroscopy (EDX), nitrogen adsorption and inverse gas chromatography (IGC), were used to check the purification protocol efficiency as well as to gather accurate information on morphology and chemical composition of diatom material obtained in large amount.展开更多
The last decade has seen a significant growth in the market for alloys used for implants,especially for those intended for orthopedic implants.Research into biodegradable magnesium-based alloys has made great strides ...The last decade has seen a significant growth in the market for alloys used for implants,especially for those intended for orthopedic implants.Research into biodegradable magnesium-based alloys has made great strides in this period,so huge progress has been made in their use in the medical industry.The important factors that led to the intensification of research in this regard,were social but also economic,wanting to improve the quality of life,by reducing the use of conventionally permanent metallic implants(stainless steel,cobalt-based alloys,and titanium alloys)which involve the second implant removal surgery and other undesirable effects(stress shielding and metal ion releases),with a negative impact on the emotional and physical condition of patients,and by significantly reducing the costs for both the patient and the health system in the field of orthopedics.This paper refers to the impact and importance of biodegradable Mg alloys,reviewing the beginning of their development,the significant characteristics that make them so desirable for such applications(orthopedic implants)but also the characteristics that must be modulated(corrosion rate and mechanical properties)to arrive at the ideal product for the targeted application.It highlights,in detail,the mechanism and aspects related to the corrosion behaviour of Mg alloys,electrochemical characterization techniques/methods,as well as strategies to improve the corrosion behaviour and mechanical properties of these types of biodegradable alloys.The means of optimization,the category and the effect of the alloying elements,the design criteria,the requirements that the implants of biodegradable alloys Mg-based must meet and the aspects related to their efficiency are also presented.Finally,the potential applications in the specialized clinics,as well as the final products currently used and made by important prestigious companies in the world are approached.展开更多
A series of Sn‐incorporated SBA‐15materials with high specific surface areas and highly orderedmesoporous structures were synthesized by a facile one‐pot method and used as catalyst supports.A reference sample was ...A series of Sn‐incorporated SBA‐15materials with high specific surface areas and highly orderedmesoporous structures were synthesized by a facile one‐pot method and used as catalyst supports.A reference sample was also prepared using a conventional impregnation method.The catalystswere characterized using various methods,and their activities in propane dehydrogenation wereinvestigated.The incorporation of Sn into the SBA‐15matrix led to strong interactions between Snspecies and the support,and these helped to maintain the oxidation states of Sn species during thereaction.Substitution with Sn changed the interfacial properties of the Pt species and improved thefunction and effect of the Sn promoter.The catalytic activities and stabilities of the Pt catalysts supportedon Sn‐incorporated SBA‐15were better than those of the impregnated sample.However,thecatalytic performance deteriorated when an excessive amount of Sn was introduced and the interactionsamong Pt,Sn species,and the support became weaker.The Pt/0.5Sn‐SBA‐15catalyst gavethe best propene selectivity,i.e.,98.5%,with a corresponding propane conversion of about43.8%.展开更多
Li4Si O4 has been regarded as one of the most promising high-temperature CO2 sorbents.However,for practical applications,its CO2sorption kinetics,cycling stability and sorption properties at lower temperatures or lowe...Li4Si O4 has been regarded as one of the most promising high-temperature CO2 sorbents.However,for practical applications,its CO2sorption kinetics,cycling stability and sorption properties at lower temperatures or lower CO2 concentrations have to be improved.In this contribution,four Li4Si O4 sorbents were synthesized from zeolite precursors MCM-41,MCM-48,TS-1,and ZSM-5.The CO2 uptake,cycling stability and the optimal CO2 sorption conditions were investigated.Among the samples,MCM-41-Li4Si O4 showed the best cycling stability at 650°C,with a stable reversible CO2 uptake of 29.1 wt%under 100 vol%CO2 during 20 cycles.But its sorption kinetics and CO2 uptakes at lower temperatures and lower CO2 concentrations need to be improved.We then demonstrated that the sorption kinetics can be improved by modifying the MCM-41 precursor with metals such as Al,Ti,Ca,and Na.The Na-MCM-41-Li4Si O4 sample exhibited the highest sorption rate,and reached the equilibrium sorption capacity close to the theoretical value of 36.7 wt%within 20 min.In addition,we proved that coating the MCM-41-Li4Si O4with Na2CO3and K2CO3can significantly increase the CO2uptakes at lower temperatures(e.g.550℃)and lower CO2concentrations(10–20 vol%).At 550℃ and under 20 vol%CO2,15 wt%K2CO3-MCM-41-Li4Si O4 and 10 wt%Na2CO3-MCM-41-Li4Si O4 sorbents resulted in a CO2 uptake of 32.2 wt%and 34.7 wt%,respectively,which are much higher than that of MCM-41-Li4Si O4(11.8 wt%).These two sorbents also showed good cycling stability.The promoiting mechasnim by alkali carbonate coating was discussed by a doubleshell model.展开更多
A hierarchical metal-free catalyst consisting of nitrogen-doped carbon nanotubes decorated onto a silicon carbide (N-CNTs/SiC) macroscopic host structure was prepared. The influence of N-CNTs incorporation on the phys...A hierarchical metal-free catalyst consisting of nitrogen-doped carbon nanotubes decorated onto a silicon carbide (N-CNTs/SiC) macroscopic host structure was prepared. The influence of N-CNTs incorporation on the physical properties of the support was evaluated using different characterization techniques. The catalyst was tested as a metal-free catalyst in the selective oxidation of H2S and steam-free dehydrogenation of ethylbenzene. The N-CNTs/SiC catalyst exhibited extremely good desulfurization performance compared to a Fe2O3/SiC catalyst under less conducive reaction conditions such as low temperature, high space velocity, and a low O2-to-H2S molar ratio. For the dehy-drogenation of ethylbenzene, a higher dehydrogenation activity was obtained with the N-CNTs/SiC catalyst compared to a commercial K-Fe/Al2O3 catalyst. The N-CNTs/SiC catalyst also displayed good stability as a function of time on stream for both reactions, which was attributed to the strong anchoring of the nitrogen dopant in the carbon matrix. The extrudate shape of the SiC support allowed the direct macroscopic shaping of the catalyst for use in a conventional fixed-bed reactor without the problems of catalyst handling, transportation, and pressure drop across the catalyst bed that are encountered with nanoscopic carbon-based catalysts.展开更多
Gold catalysis had been considered a highly efficient candidate for heterogeneous catalysis.It is well established that reducible-material-supported Au NPs are more reactive than the unreducible materials,unless speci...Gold catalysis had been considered a highly efficient candidate for heterogeneous catalysis.It is well established that reducible-material-supported Au NPs are more reactive than the unreducible materials,unless specific modifications are carried out.However,unreducible materials such as carbon materials,silica,and alumina have particular advantages,including the easily controlled surface property,adjustable microscopic structure,earth-abundant reserves,and facile industrial manufacture.New strategies,influences,and mechanisms of modification to enhance the catalytic performance and thermal stability of unreducible-material-supported gold catalysts are among the most attractive research topics in gold catalysis.However,to the best of our knowledge,reports and reviews focused on unreducible-material-supported gold catalysts are lacking.Herein,the above concept will be thoroughly discussed regarding several typical unreducible supports,including the commonly used silica,alumina,carbon materials,and hydroxyapatite.The currently prevailing modification strategies will be summarized in detail from the aspects of theoretical conceptualization and practical methodology,including the ingenious synthesis method for catalyst with a specific structure,the currently prosperous electrostatic adsorption,colloid immobilization,and the applicative thermal gaseous treatment.The influences of physical and chemical modifications on the surface chemistry,electronic structure,interaction/synergy between Au-support/promoter,catalyst morphology and water precipitation will be also summarized.It is assumed that the review will shed light on significant studies on unreducible support in gold catalysis with the purpose of catalytic promotion and the promotion of the potential industrial demands in advance.Furthermore,the review will provide new insights into unreducible supports that can be potentially applied in gold catalysis.展开更多
Undoped nickel-based catalysts supported on depleted uranium oxide allow one to carry out CO_(2)methanation process under extremely low reaction temperature under atmospheric pressure and powered by a contactless indu...Undoped nickel-based catalysts supported on depleted uranium oxide allow one to carry out CO_(2)methanation process under extremely low reaction temperature under atmospheric pressure and powered by a contactless induction heating.By adjusting the reaction conditions,the catalyst is able to perform CO_(2)methanation reaction under autothermal process operated inside a non-adiabatic reactor,without any external energy supply.Such autothermal process is possible thanks to the high apparent density of the UO_x which allows one to confine the reaction heat in a small catalyst volume in order to confine the exothermicity of the reaction inside the catalyst and to operate the reaction at equilibrium heat in-heat out.Such autothermal operation mode allows one to significantly reduce the complexity of the process compared to that operated using adiabatic reactor,where complete insulation is required to prevent heat disequilibrium,in order to reduce as much as possible,the heat exchange with the external medium.The catalyst displays an extremely high stability as a function of time on stream as no apparent deactivation.It is expected that such new catalyst with unprecedented catalytic performance could open new era in the field of heterogeneous catalysis where traditional supports show their limitations to operate catalytic processes under severe reaction conditions.展开更多
Bimetallic Au_xCu_y/CeO_2（x/y = 3/1,1/1,and 1 /3） catalysts were prepared by direct anion exchange（DAE）,following impregnation（IMP） methods,and used for selective hydrogenation of cinnamaldehyde.The effects of p...Bimetallic Au_xCu_y/CeO_2（x/y = 3/1,1/1,and 1 /3） catalysts were prepared by direct anion exchange（DAE）,following impregnation（IMP） methods,and used for selective hydrogenation of cinnamaldehyde.The effects of pretreatments,such as calcination or reduction on the catalytic activities of these catalysts were investigated.XRD and HRTEM showed that for the reduced catalysts,there is the formation of an Au-Cu alloy.HAADF-STEM displayed that reduction pretreatment leads to a very homogenous distribution of Au and Cu on the external catalyst surface.Reaction parameters,such as CAL concentration,the stirring speed,nature of the solvent influence the catalytic activities.Pretreatments lead to a major effect on CAL conversion and HCAL selectivity.Catalysts Au_xCu_y/CeO_2 pretreated under reduction display higher CAL conversion and HCAL selectivity than that of under calcination mainly due to the synergistic effect resulting in a formation of Au-Cu alloy.展开更多
Photocatalytic degradation of paraquat (PQ) aqueous solutions was studied in a fixed bed photoreactor under UV irradiation at 368 nm. This contained β-SiC alveolar foams coated with TiO2 P25 by dip-coating method. SE...Photocatalytic degradation of paraquat (PQ) aqueous solutions was studied in a fixed bed photoreactor under UV irradiation at 368 nm. This contained β-SiC alveolar foams coated with TiO2 P25 by dip-coating method. SEM analyses revealed that the surface of the film did not exhibit cracks in the presence of TTIP as a binder in the TiO2 P25 suspension. The following parameters were studied in continuous mode operation: the flow rate in the reactor, the initial concentration of the paraquat, the pH of the solution, the weight of photocatalytic material with the number of foams in the reactor and the weight of the catalyst deposited onto the support. The results showed that by working under optimal operating conditions at natural pH (pH = 6.7), low paraquat (Co = 10 ppm), and flow (26 mL/min), we recorded approximately (43.16 ± 1.00)% oxidation of paraquat and a decrease in total organic carbon (TOC) of (27.13 ± 1.00)% after about 70 minutes. The apparent rate constant is in the order of (0.0656 ± 0.0010) min-1. In addition, by increasing the amount of β-SiC foams coated with TiO2, we improve the degradation of paraquat in the same order. The study of aging of the material showed its stability over time. However, photocatalytic activity was limited after 20 minutes of UV irradiation due to the limitation of the diffusion of the paraquat molecules towards the surface of the photocatalyst. As an outcome, we obtained an efficient TiO2/β-SiC material for photocatalytic degradation of organic compounds in water.展开更多
Gasification experiments were carried out in a pilot scale fluid bed reactor operated under allothermal mode and low fluidisation regime with iron-doped olivine and char as catalyst for in-situ tar abatement.The catal...Gasification experiments were carried out in a pilot scale fluid bed reactor operated under allothermal mode and low fluidisation regime with iron-doped olivine and char as catalyst for in-situ tar abatement.The catalyst combination resulted in a reduction of 50%in the overall tar yield with respect to the reference values.Furthermore,the integration of an oxidative Hot Gas Filtration unit downstream the gasification reactor led to a further reduction in overall tar yield and relatively clean gas was obtained(approx.1 g/Nm3,benzene-free).The tar dew point of the resulting producer gas was estimated to 80℃,only 40℃ above the threshold value recommended for its valorisation in standard internal combustion engines.Moreover,catalyst elutriation and char hold-up took place to a large extent inside the reactor.The analysis of catalyst samples at different Time-On-Stream(TOS)revealed:(i)a considerable loss of iron oxides during the first hour of test because of the interparticle mechanical attrition(mostly surface abrasion)and partial reduction of hematite to magnetite and wustite but,stable composition at higher TOS,(ii)the loss of the iron oxide coverage of Fe/olivine particles and the formation of agglomerates with increasing TOS and,(iii)the amount of carbon deposited in the surface of the Fe/olivine particles increased with TOS,but in any case,these carbon deposits can be completely oxidized above 650℃.展开更多
The use of non-noble nickel-based catalysts for low temperature CO methanation has been a challenge in recent years.Herein,MgAl layered double oxides sample with high dispersion synthesized by a facile N-(2-Hydroxyeth...The use of non-noble nickel-based catalysts for low temperature CO methanation has been a challenge in recent years.Herein,MgAl layered double oxides sample with high dispersion synthesized by a facile N-(2-Hydroxyethyl)ethylenediaminetriacetic acid assisted wetness impregnation approach,demonstrates much superior catalytic activity and exceptional stability for CO methanation in comparison with the classical Ni/MgAl-LDO catalyst prepared by the ordinary wetness impregnation method.HRTEM results showed that N-(2-Hydroxyethyl)ethylenediaminetriacetic acid played a positive role in the dispersion of Ni,as well as Ni-support interaction.Well-dispersed Ni particles with a size of about 5 nm were formed in the presence of N-(2-Hydroxyethyl)ethylenediaminetriacetic acid.Compared to the Ni/MgAl-LDO prepared by conventional impregnation method,the NH-Ni/MgAl-LDO exhibited superior catalytic performance,especially excellent thermal stability.The NH-Ni30/MgAl-LDO catalyst was found to keep a 70%CO conversion even at 160◦C which demonstrates its good low temperature performance.From the in situ FTIR observations,this good performance at low temperatures may be linked to the delocalization of electrons around CO caused by surface hydroxyl groups.展开更多
文摘Bio-silica issued from diatom, a microalgae, is attracted increasing attention in material science thanks to its peculiar nanoarchitecture and related properties with versatile applications. The present work is a deep analysis on morphological and chemical properties of bio-silica issued from fossil origin (diatomaceous earth) and living one (algal paste). An optimization in purification protocol was performed to obtain multiparous bio-silica from its raw media with keeping its original shape entirely. Multiple characterization methods as scanning electronic microscopy (SEM), infrared spectroscopy, x-ray diffraction (DRX), X-ray photoelectron spectroscopy (XPS), energy dispersive X-ray spectroscopy (EDX), nitrogen adsorption and inverse gas chromatography (IGC), were used to check the purification protocol efficiency as well as to gather accurate information on morphology and chemical composition of diatom material obtained in large amount.
基金performed under contracts no.46N/2019-project no.PN19310102/2019 and 30PFE/2018 between the National Institute for Research and Development in Electrical Engineering ICPE-CA and the Romanian Ministry of Research and Innovation
文摘The last decade has seen a significant growth in the market for alloys used for implants,especially for those intended for orthopedic implants.Research into biodegradable magnesium-based alloys has made great strides in this period,so huge progress has been made in their use in the medical industry.The important factors that led to the intensification of research in this regard,were social but also economic,wanting to improve the quality of life,by reducing the use of conventionally permanent metallic implants(stainless steel,cobalt-based alloys,and titanium alloys)which involve the second implant removal surgery and other undesirable effects(stress shielding and metal ion releases),with a negative impact on the emotional and physical condition of patients,and by significantly reducing the costs for both the patient and the health system in the field of orthopedics.This paper refers to the impact and importance of biodegradable Mg alloys,reviewing the beginning of their development,the significant characteristics that make them so desirable for such applications(orthopedic implants)but also the characteristics that must be modulated(corrosion rate and mechanical properties)to arrive at the ideal product for the targeted application.It highlights,in detail,the mechanism and aspects related to the corrosion behaviour of Mg alloys,electrochemical characterization techniques/methods,as well as strategies to improve the corrosion behaviour and mechanical properties of these types of biodegradable alloys.The means of optimization,the category and the effect of the alloying elements,the design criteria,the requirements that the implants of biodegradable alloys Mg-based must meet and the aspects related to their efficiency are also presented.Finally,the potential applications in the specialized clinics,as well as the final products currently used and made by important prestigious companies in the world are approached.
基金supported by the Science & Technology Support Plan Projects of Sichuan Province (2016GZ0371)National Natural Science Foun-dation of China (NNSFC,21476145,21506111)~~
文摘A series of Sn‐incorporated SBA‐15materials with high specific surface areas and highly orderedmesoporous structures were synthesized by a facile one‐pot method and used as catalyst supports.A reference sample was also prepared using a conventional impregnation method.The catalystswere characterized using various methods,and their activities in propane dehydrogenation wereinvestigated.The incorporation of Sn into the SBA‐15matrix led to strong interactions between Snspecies and the support,and these helped to maintain the oxidation states of Sn species during thereaction.Substitution with Sn changed the interfacial properties of the Pt species and improved thefunction and effect of the Sn promoter.The catalytic activities and stabilities of the Pt catalysts supportedon Sn‐incorporated SBA‐15were better than those of the impregnated sample.However,thecatalytic performance deteriorated when an excessive amount of Sn was introduced and the interactionsamong Pt,Sn species,and the support became weaker.The Pt/0.5Sn‐SBA‐15catalyst gavethe best propene selectivity,i.e.,98.5%,with a corresponding propane conversion of about43.8%.
基金supported by the National Natural Science Foundation of China (51622801, 51572029)Beijing Excellent Young Scholar (2015000026833ZK11)the Beijing Natural Science Foundation (2184114)
文摘Li4Si O4 has been regarded as one of the most promising high-temperature CO2 sorbents.However,for practical applications,its CO2sorption kinetics,cycling stability and sorption properties at lower temperatures or lower CO2 concentrations have to be improved.In this contribution,four Li4Si O4 sorbents were synthesized from zeolite precursors MCM-41,MCM-48,TS-1,and ZSM-5.The CO2 uptake,cycling stability and the optimal CO2 sorption conditions were investigated.Among the samples,MCM-41-Li4Si O4 showed the best cycling stability at 650°C,with a stable reversible CO2 uptake of 29.1 wt%under 100 vol%CO2 during 20 cycles.But its sorption kinetics and CO2 uptakes at lower temperatures and lower CO2 concentrations need to be improved.We then demonstrated that the sorption kinetics can be improved by modifying the MCM-41 precursor with metals such as Al,Ti,Ca,and Na.The Na-MCM-41-Li4Si O4 sample exhibited the highest sorption rate,and reached the equilibrium sorption capacity close to the theoretical value of 36.7 wt%within 20 min.In addition,we proved that coating the MCM-41-Li4Si O4with Na2CO3and K2CO3can significantly increase the CO2uptakes at lower temperatures(e.g.550℃)and lower CO2concentrations(10–20 vol%).At 550℃ and under 20 vol%CO2,15 wt%K2CO3-MCM-41-Li4Si O4 and 10 wt%Na2CO3-MCM-41-Li4Si O4 sorbents resulted in a CO2 uptake of 32.2 wt%and 34.7 wt%,respectively,which are much higher than that of MCM-41-Li4Si O4(11.8 wt%).These two sorbents also showed good cycling stability.The promoiting mechasnim by alkali carbonate coating was discussed by a doubleshell model.
基金financially supported by a European project (FREECATS) under a contract number NMP-2011-2.2-4 "Novel materials for replacement of strategic or scarce raw materials"
文摘A hierarchical metal-free catalyst consisting of nitrogen-doped carbon nanotubes decorated onto a silicon carbide (N-CNTs/SiC) macroscopic host structure was prepared. The influence of N-CNTs incorporation on the physical properties of the support was evaluated using different characterization techniques. The catalyst was tested as a metal-free catalyst in the selective oxidation of H2S and steam-free dehydrogenation of ethylbenzene. The N-CNTs/SiC catalyst exhibited extremely good desulfurization performance compared to a Fe2O3/SiC catalyst under less conducive reaction conditions such as low temperature, high space velocity, and a low O2-to-H2S molar ratio. For the dehy-drogenation of ethylbenzene, a higher dehydrogenation activity was obtained with the N-CNTs/SiC catalyst compared to a commercial K-Fe/Al2O3 catalyst. The N-CNTs/SiC catalyst also displayed good stability as a function of time on stream for both reactions, which was attributed to the strong anchoring of the nitrogen dopant in the carbon matrix. The extrudate shape of the SiC support allowed the direct macroscopic shaping of the catalyst for use in a conventional fixed-bed reactor without the problems of catalyst handling, transportation, and pressure drop across the catalyst bed that are encountered with nanoscopic carbon-based catalysts.
文摘Gold catalysis had been considered a highly efficient candidate for heterogeneous catalysis.It is well established that reducible-material-supported Au NPs are more reactive than the unreducible materials,unless specific modifications are carried out.However,unreducible materials such as carbon materials,silica,and alumina have particular advantages,including the easily controlled surface property,adjustable microscopic structure,earth-abundant reserves,and facile industrial manufacture.New strategies,influences,and mechanisms of modification to enhance the catalytic performance and thermal stability of unreducible-material-supported gold catalysts are among the most attractive research topics in gold catalysis.However,to the best of our knowledge,reports and reviews focused on unreducible-material-supported gold catalysts are lacking.Herein,the above concept will be thoroughly discussed regarding several typical unreducible supports,including the commonly used silica,alumina,carbon materials,and hydroxyapatite.The currently prevailing modification strategies will be summarized in detail from the aspects of theoretical conceptualization and practical methodology,including the ingenious synthesis method for catalyst with a specific structure,the currently prosperous electrostatic adsorption,colloid immobilization,and the applicative thermal gaseous treatment.The influences of physical and chemical modifications on the surface chemistry,electronic structure,interaction/synergy between Au-support/promoter,catalyst morphology and water precipitation will be also summarized.It is assumed that the review will shed light on significant studies on unreducible support in gold catalysis with the purpose of catalytic promotion and the promotion of the potential industrial demands in advance.Furthermore,the review will provide new insights into unreducible supports that can be potentially applied in gold catalysis.
基金ORANO Chimie-Enrichissement Co.for the financial support of this project。
文摘Undoped nickel-based catalysts supported on depleted uranium oxide allow one to carry out CO_(2)methanation process under extremely low reaction temperature under atmospheric pressure and powered by a contactless induction heating.By adjusting the reaction conditions,the catalyst is able to perform CO_(2)methanation reaction under autothermal process operated inside a non-adiabatic reactor,without any external energy supply.Such autothermal process is possible thanks to the high apparent density of the UO_x which allows one to confine the reaction heat in a small catalyst volume in order to confine the exothermicity of the reaction inside the catalyst and to operate the reaction at equilibrium heat in-heat out.Such autothermal operation mode allows one to significantly reduce the complexity of the process compared to that operated using adiabatic reactor,where complete insulation is required to prevent heat disequilibrium,in order to reduce as much as possible,the heat exchange with the external medium.The catalyst displays an extremely high stability as a function of time on stream as no apparent deactivation.It is expected that such new catalyst with unprecedented catalytic performance could open new era in the field of heterogeneous catalysis where traditional supports show their limitations to operate catalytic processes under severe reaction conditions.
基金the Chinese Scholarship Council (CSC), French Eiffel Scholarship for financial supports of Xuemei Liaothe financial supported by the Open Research Subject of key laboratory (Research Base) of Grain and Oil Engineering and food safety (No. szjj2015-006)Agricultural and Forestry Talents in Food quality and safety, Key Research Fund of Xihua University (No. Z1520527)
文摘Bimetallic Au_xCu_y/CeO_2（x/y = 3/1,1/1,and 1 /3） catalysts were prepared by direct anion exchange（DAE）,following impregnation（IMP） methods,and used for selective hydrogenation of cinnamaldehyde.The effects of pretreatments,such as calcination or reduction on the catalytic activities of these catalysts were investigated.XRD and HRTEM showed that for the reduced catalysts,there is the formation of an Au-Cu alloy.HAADF-STEM displayed that reduction pretreatment leads to a very homogenous distribution of Au and Cu on the external catalyst surface.Reaction parameters,such as CAL concentration,the stirring speed,nature of the solvent influence the catalytic activities.Pretreatments lead to a major effect on CAL conversion and HCAL selectivity.Catalysts Au_xCu_y/CeO_2 pretreated under reduction display higher CAL conversion and HCAL selectivity than that of under calcination mainly due to the synergistic effect resulting in a formation of Au-Cu alloy.
文摘Photocatalytic degradation of paraquat (PQ) aqueous solutions was studied in a fixed bed photoreactor under UV irradiation at 368 nm. This contained β-SiC alveolar foams coated with TiO2 P25 by dip-coating method. SEM analyses revealed that the surface of the film did not exhibit cracks in the presence of TTIP as a binder in the TiO2 P25 suspension. The following parameters were studied in continuous mode operation: the flow rate in the reactor, the initial concentration of the paraquat, the pH of the solution, the weight of photocatalytic material with the number of foams in the reactor and the weight of the catalyst deposited onto the support. The results showed that by working under optimal operating conditions at natural pH (pH = 6.7), low paraquat (Co = 10 ppm), and flow (26 mL/min), we recorded approximately (43.16 ± 1.00)% oxidation of paraquat and a decrease in total organic carbon (TOC) of (27.13 ± 1.00)% after about 70 minutes. The apparent rate constant is in the order of (0.0656 ± 0.0010) min-1. In addition, by increasing the amount of β-SiC foams coated with TiO2, we improve the degradation of paraquat in the same order. The study of aging of the material showed its stability over time. However, photocatalytic activity was limited after 20 minutes of UV irradiation due to the limitation of the diffusion of the paraquat molecules towards the surface of the photocatalyst. As an outcome, we obtained an efficient TiO2/β-SiC material for photocatalytic degradation of organic compounds in water.
基金the ADEME,France(Adelither-project N◦1702C0042)the Region Grand-Est,France(Feder Project Hy-C-Green)for the financial support.
文摘Gasification experiments were carried out in a pilot scale fluid bed reactor operated under allothermal mode and low fluidisation regime with iron-doped olivine and char as catalyst for in-situ tar abatement.The catalyst combination resulted in a reduction of 50%in the overall tar yield with respect to the reference values.Furthermore,the integration of an oxidative Hot Gas Filtration unit downstream the gasification reactor led to a further reduction in overall tar yield and relatively clean gas was obtained(approx.1 g/Nm3,benzene-free).The tar dew point of the resulting producer gas was estimated to 80℃,only 40℃ above the threshold value recommended for its valorisation in standard internal combustion engines.Moreover,catalyst elutriation and char hold-up took place to a large extent inside the reactor.The analysis of catalyst samples at different Time-On-Stream(TOS)revealed:(i)a considerable loss of iron oxides during the first hour of test because of the interparticle mechanical attrition(mostly surface abrasion)and partial reduction of hematite to magnetite and wustite but,stable composition at higher TOS,(ii)the loss of the iron oxide coverage of Fe/olivine particles and the formation of agglomerates with increasing TOS and,(iii)the amount of carbon deposited in the surface of the Fe/olivine particles increased with TOS,but in any case,these carbon deposits can be completely oxidized above 650℃.
基金National Natural Science Foundation of China(No.22068034)International Science and Technology Cooperation Project of Shihezi University(No.GJHZ201804)+1 种基金International Science and Technology Cooperation Project of Bingtuan(No.2018BC002)Science and Technology Innovation Talents Program of Bingtuan(No.2019CB025).
文摘The use of non-noble nickel-based catalysts for low temperature CO methanation has been a challenge in recent years.Herein,MgAl layered double oxides sample with high dispersion synthesized by a facile N-(2-Hydroxyethyl)ethylenediaminetriacetic acid assisted wetness impregnation approach,demonstrates much superior catalytic activity and exceptional stability for CO methanation in comparison with the classical Ni/MgAl-LDO catalyst prepared by the ordinary wetness impregnation method.HRTEM results showed that N-(2-Hydroxyethyl)ethylenediaminetriacetic acid played a positive role in the dispersion of Ni,as well as Ni-support interaction.Well-dispersed Ni particles with a size of about 5 nm were formed in the presence of N-(2-Hydroxyethyl)ethylenediaminetriacetic acid.Compared to the Ni/MgAl-LDO prepared by conventional impregnation method,the NH-Ni/MgAl-LDO exhibited superior catalytic performance,especially excellent thermal stability.The NH-Ni30/MgAl-LDO catalyst was found to keep a 70%CO conversion even at 160◦C which demonstrates its good low temperature performance.From the in situ FTIR observations,this good performance at low temperatures may be linked to the delocalization of electrons around CO caused by surface hydroxyl groups.
