Wet flue gas desulfurization(WFGD)could effectively reduce sulfur dioxide emission.However,magnesium sulfite(MgSO_(3)),a by-product of desulfurization,was easy to result in secondary pollution.In this study,the solid ...Wet flue gas desulfurization(WFGD)could effectively reduce sulfur dioxide emission.However,magnesium sulfite(MgSO_(3)),a by-product of desulfurization,was easy to result in secondary pollution.In this study,the solid catalyst Co-Bent(bentonite supported cobalt)was prepared by blending method for MgSO_(3) oxidation with bentonite as the carrier and cobalt as the active component.At the calcination temperature of 550℃ and the Co loading level of 3 wt.%,the catalyst showed excellent catalytic performance for the oxidation of high concentration MgSO_(3) slurry,and the oxidation rate of MgSO_(3) was 0.13 mol/(L·h).The research indicated that the active component was uniformly distributed within porous structure of the catalyst as Co_(3)O_(4),which facilitated the oxidation of SO_(3)^(2-) catalyzed by Co_(3)O_(4).Kinetic researches indicated the oxidation rate of MgSO_(3) was influenced by the catalyst dosage,the reaction temperature,the solution pH,the airflow rate,and the SO_(3)^(2-) concentration.Additionally,after recycling experiments,the regenerated catalyst retained its high catalytic performance for the MgSO_(3) oxidation.The reaction mechanism for the catalytic oxidation of MgSO_(3) by Co-Bent catalyst was also proposed.The generation of active free radicals(OH·,SO_(4)^(-)·,SO_(3)^(-)·,SO_(5)^(-)·)accelerated the MgSO_(3) oxidation.These results provide theoretical support for the treatment of MgSO_(3) and the development of durable catalyst.展开更多
Perovskite oxides LaCoO3 prepared by templating,co-precipitation and sol-gel method with different complexants were systematically characterized and its catalytic performances for CO oxidation were investigated.The sa...Perovskite oxides LaCoO3 prepared by templating,co-precipitation and sol-gel method with different complexants were systematically characterized and its catalytic performances for CO oxidation were investigated.The samples were characterized by X-ray diffraction,thermogravimetry analysis and differential scanning calorimetry,N2 physisorption,transmission electron microscopy,temperature program reduction of hydrogen,temperature program desorption of oxygen and X-ray photoelectron spectroscopy measurement,results of which show that the properties of LaCoO3,such as surface morphology,surface area,surface compositions,redox capability,oxygen vacancy,as well as the calcination temperature and formation mechanism,depend intimately on the preparation method.Catalytic tests indicate that the sample prepared by carbon templating method shows the best activity for CO oxidation,with full CO conversion obtained at 135℃.In particular,the catalyst can be activated and significant increase of activity can be obtained with the increase of reaction time.The cyclic and longterm stability of catalysts were discussed and compared.展开更多
Influence of three different preparation methods, i.e. impregnation, coprecipitation, and inverse coprecipitation, on the preferential oxidation of CO in excess hydrogen （PROX） over CuO-CeO2 catalysts has been inves...Influence of three different preparation methods, i.e. impregnation, coprecipitation, and inverse coprecipitation, on the preferential oxidation of CO in excess hydrogen （PROX） over CuO-CeO2 catalysts has been investigated and CuO-CeO2 catalysts are characterized using BET, XPS, XRD, UV Raman, and TPR techniques. The results show that the catalysts prepared by coprecipitation have smaller particle sizes, well-dispersed CuOx species, more oxygen vacancies, and are more active in the PROX than those prepared by the other methods. However. the inverse coprecipitation depresses the catalytic performance of CuO-CeO2 catalysts and causes the growth of CuO-CeO2 because of different pH value in the precipitation process.展开更多
A series of SnO2‐based catalysts modified by Mn, Zr, Ti and Pb oxides with a Sn/M （M=Mn, Zr, Ti and Pb） molar ratio of 9/1 were prepared by a co‐precipitation method and used for CH4 and CO oxidation. The Mn3＋, ...A series of SnO2‐based catalysts modified by Mn, Zr, Ti and Pb oxides with a Sn/M （M=Mn, Zr, Ti and Pb） molar ratio of 9/1 were prepared by a co‐precipitation method and used for CH4 and CO oxidation. The Mn3＋, Zr4＋, Ti4＋and Pb4＋cations are incorporated into the lattice of tetragonal rutile SnO2 to form a solid solution structure. As a consequence, the surface area and thermal stability of the catalysts are improved. Moreover, the oxygen species of the modified catalysts become easier to be reduced. Therefore, the oxidation activity over the catalysts was improved, except for the one modified by Pb oxide. Manganese oxide demonstrates the best promotional effects for SnO2. Using an X‐ray diffraction extrapolation method, the lattice capacity of SnO2 for Mn2O3 was 0.135 g Mn2O3/g SnO2, which indicates that to form stable solid solution, only 21%Sn4＋cations in the lattice can be maximally replaced by Mn3＋. If the amount of Mn3＋cations is over the capacity, Mn2O3 will be formed, which is not favorable for the activity of the catalysts. The Sn rich samples with only Sn‐Mn solid solution phase show higher activity than the ones with excess Mn2O3 species.展开更多
Based on the demand of sintering/pelleting flue gas ultra-low emission,a semi-dry method using a spray dryer absorber (SDA) combined with O3 oxidation was proposed for simultaneous removal of SO2 and NO.Effects of O3 ...Based on the demand of sintering/pelleting flue gas ultra-low emission,a semi-dry method using a spray dryer absorber (SDA) combined with O3 oxidation was proposed for simultaneous removal of SO2 and NO.Effects of O3 injection site,O3/NO molar ratio,and spray tower temperature on the removal efficiencies were investigated.It was revealed that both desulfurization and denitrification efficiencies could reach to 85%under the conditions of setting O3 injection site inside of tower,O3/NO molar ratio 1.8,spray tower temperature 85°C,Ca/(S+2N) molar ratio 2.5 and slurry flow rate 300 m L/hr.CaSO3/Ca(OH)2 mixture slurry was used as absorbent to simulate operating conditions in iron and steel industry.The result shows that the addition of CaSO3 weakens both removal efficiencies.In addition,the reaction mechanism of simultaneous removal of SO2 and NO using SDA combined with O3 oxidation was proposed.展开更多
Facile green oxidation methods are always desired to functionalize carbon nanotubes(CNTs)in the production of advanced CNT/epoxy composites.In the present work,an optimized H2O2/H2O/O3 oxidation method was developed,a...Facile green oxidation methods are always desired to functionalize carbon nanotubes(CNTs)in the production of advanced CNT/epoxy composites.In the present work,an optimized H2O2/H2O/O3 oxidation method was developed,and performances of the H2O2/H2O/O3 oxidized CNT in epoxy matrix were tested and compared with that of the H2O/O3 oxidized CNT and the most commonly used concentrated HNO3 oxidized CNT.The physical and chemical characteristics of the obtained oxidized CNTs were systematically characterized via transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS)and Raman.Mechanical performances of the obtained composites were explored by tensile tests,impact tests,dynamic mechanical analysis(DMA)and fracture toughness tests.It was found that the H2O2/H2O/O3 oxidized CNT exhibited all-around overwhelming advantages over the concentrated HNO3 oxidized CNT on reinforcing the epoxy matrix,while the H2O/O3 oxidized CNT only improved the material strength.Reinforcing mechanisms for the different methods oxidized CNTs were studied and compared.The optimized H2O2/H2O/O3 oxidation method makes scaled production possible,avoids environment pollutions,and holds great potentials to replace the most commonly used concentrated HNO3 oxidation method to oxidize CNT during the preparation of the advanced CNT/epoxy composite.展开更多
With the vigorous development of China's iron and steel industry and the introduction of ultra-low emission policies,the emission of pollutants such as SO_(2)and NO x has received unprecedented attention.Consideri...With the vigorous development of China's iron and steel industry and the introduction of ultra-low emission policies,the emission of pollutants such as SO_(2)and NO x has received unprecedented attention.Considering the increase of the proportion of semi-dry desulfurization technology in the desulfurization process,several semi-dry desulphurization technologies such as flue gas circulating fluidized bed(CFB),dense flow absorber(DFA)and spray drying absorption(SDA)are briefly summarized.Moreover,a method for simultaneous treatment of SO_(2)and NOx in sintering/pelletizing flue gas by O_(3)oxidation combined with semidry method is introduced.Meantime,the effects of key parameters such as O_(3)/NO molar ratio,Ca SO_(3),SO_(2),reaction temperature,Ca/(S+2 N)molar ratio,droplet size and approach to adiabatic saturation temperature(AAST)on denitrification and desulfurization are analyzed.Furthermore,the reaction mechanism of denitrification and desulfurization is further elucidated.Finally,the advantages and development prospects of the new technology are proposed.展开更多
The Cu-Zr-Ce-O catalysts prepared using the coprecipitation method exhibited better catalytic performance for CO selective oxidation. The Cu-Zr-Ce-O catalysts pretreated with different methods were studied by CO-TPR a...The Cu-Zr-Ce-O catalysts prepared using the coprecipitation method exhibited better catalytic performance for CO selective oxidation. The Cu-Zr-Ce-O catalysts pretreated with different methods were studied by CO-TPR and XPS techniques. The results showed that the Cu-Zr-Ce-O catalyst pretreated with oxygen exhibited the best catalytic performance and had the widest operating temperature window, with CO conversion above 99% from 160 to 200 ℃. The O2 pretreatment caused an enrichment of the oxygen storaged on the Cu active species and promoted the conversion of adsorbed oxygen into surface lattice oxygen. It also improved the amount of Cu＋/Cu^2＋ ionic pair, and then facilitated the formation of CuO active species on the catalyst for selective CO oxidation.展开更多
The removal of hydrogen sulfide from gas plays an important role in rational utilization of resources and environ- mental protection. In this paper, the process of hydrogen sulfide removal by wet oxidation method in a...The removal of hydrogen sulfide from gas plays an important role in rational utilization of resources and environ- mental protection. In this paper, the process of hydrogen sulfide removal by wet oxidation method in a rotating packed bed was investigated in a scale for treating 10 000 Nm3/h of gas. On the basis of studying the influence of the species and con- centration of alkali source, the liquid/gas volume ratio, the high gravity factor, and the hydrogen sulfide content in feed gas on the desulfurization effect, the suitable technological conditions were obtained. The hydrogen sulfide removal efficiency could reach 98.0% under these conditions. The results of continuous operation of process facilities showed that the high gravity method has many merits including higher desulfurization rate, good stability in operation, lower liquid/gas volume ratio, greater operation elasticity, and apparent energy saving effects.展开更多
A novel and convenient hydrolysis and oxidation method was first used in preparation of carbon contained Y2O3 phosphor powders. The alloy was hydrolyzed in deionized water and the obtained Y（OH）3 powders were heat t...A novel and convenient hydrolysis and oxidation method was first used in preparation of carbon contained Y2O3 phosphor powders. The alloy was hydrolyzed in deionized water and the obtained Y（OH）3 powders were heat treated in air atmosphere. The final products - Y2O3 powders were micron clusters which were aggregated by hundreds of nanoparticles with the size of about 5 nm. The chemical composition, structural and morphological features of the samples were characterized by means of X-ray powder diffraction （XRD） analysis, transmission electron microscopy （TEM）, Fourier-transform infrared （FT-IR） spectra, X-ray photoelectron spectra （XPS） and carbon sulfur analyzer. The obtained powders showed good bluish-white photoluminescence （PL） emissions （ranging from 430 to 600 nm, peaking at 468 nm and 578 nm） under the xenon light excitation. The luminescent mechanism was ascribed to the carbon impurities in the Y2O3 host.展开更多
The CuO-CeO2 catalyst prepared by chelating method has a superior catalytic performance for the preferential oxidation of CO in rich hydrogen, compared with the CuO-CeO2 catalyst prepared by coprecipitation method. Th...The CuO-CeO2 catalyst prepared by chelating method has a superior catalytic performance for the preferential oxidation of CO in rich hydrogen, compared with the CuO-CeO2 catalyst prepared by coprecipitation method. The CO conversions over these catalysts, at 120 ℃ and 120000 ml/（g-h） in the absence of CO2 and H2O, are 99.6% and 88.6%, respectively, and the selectivity of O2 over these catalysts is very close （i.e. 51.3% and 55.8%, respectively）. The influence of certain factors such as hydrogen concentration, carbon monoxide concentration, H2O, O2/CO ratios, and space velocity on the catalytic performance of CuO-CeO2 catalyst prepared by chelating method is also studied. The results show that the addition of hydrogen and H2O has a negative effect on the catalytic performance of CuO-CeO2 catalyst, however, the variation of space velocity and the O2/CO ratio causes a comparatively slight influence.展开更多
We adopted the solution impregnation route with aluminum dihydrogen phosphate solution as liquid medium for effective surface modification on graphite substrate.The mass ratio of graphite to Al(H_(2)PO_(4))_(3) change...We adopted the solution impregnation route with aluminum dihydrogen phosphate solution as liquid medium for effective surface modification on graphite substrate.The mass ratio of graphite to Al(H_(2)PO_(4))_(3) changed from 0.5:1 to 4:1,and the impregnation time changed from 1 to 7 h.The typical composite phase change thermal storage materials doped with the as-treated graphite were fabricated using form-stable technique.To investigate the oxidation and anti-oxidation behavior of the impregnated graphite at high temperatures,the samples were put into a muffle furnace for a cyclic heat test.Based on SEM,EDS,DSC techniques,analyses on the impregnated technique suggested an optimized processing conditions of a 3 h impregnation time with the ratio of graphite:Al(H_(2)PO_(4))_(3) as 1:3 for graphite impregnation treatment.Further investigations on high-temperature phase change heat storage materials doped by the treated graphite suggested excellent oxidation resistance and thermal cycling performance.展开更多
High-temperature oxidation is an important property to evaluate thermal protection materials. However, since oxidation is a complex process involving microstructure evolution, its quantitative analysis has always been...High-temperature oxidation is an important property to evaluate thermal protection materials. However, since oxidation is a complex process involving microstructure evolution, its quantitative analysis has always been a challenge. In this work, a phase field method （PFM） based on the thermodynamics theory is developed to simulate the oxidation behavior and oxidation induced growth stress. It involves microstructure evolution and solves the problem of quantitatively computational analysis for the oxidation behavior and growth stress. Employing this method, the diffusion process, oxidation performance, and stress evolution axe predicted for Fe-Cr-A1-Y alloys. The numerical results agree well with the experimental data. The linear relationship between the maximum growth stress and the environment oxygen concentration is found. PFM provides a powerful tool to investigate high-temperature oxidation in complex environments.展开更多
The influence of different cooking and smoking methods (boiling, frying, frying + boiling, hot and cold smoking) on oxidation and fatty acid composition of catfish (Arius maculatus) commercialized on the Wouri river c...The influence of different cooking and smoking methods (boiling, frying, frying + boiling, hot and cold smoking) on oxidation and fatty acid composition of catfish (Arius maculatus) commercialized on the Wouri river coast was evaluated including commonly used analytical indexes (peroxide and acid values)and physical analysis by Fourier transform infrared (FTIR) spectroscopy. The mean moisture, protein, ash and fat contents of raw fish were 75.88 ± 0.55;64.24 ± 0.14;10.98 ± 0.31 and 23.02 ± 0.88 respectively. All these treatments provoke the modification of the quality indexes. Lipid deterioration, thermolysis and lipid oxidation occurred throughout the treatment. Peroxide value decreased for all cooked and smoked catfish, while free fatty acids of smoked sample increased. The FTIR applied to evaluate lipid oxidation in extracted lipid clearly provided a better picture of the oxidation progress and led to a similar conclusion with chemical analysis. Boiled, bleaching hot and bleaching cold smoking were found to be the suitable treatment methods for catfish because they gave it a high nutritive value compared to other smoking methods.展开更多
In this paper,the CuO-CeO_(2) catalyst was prepared by a direct solvothermal method.The effects of different copper salt precursors(copper nitrate,copper acetate,copper sulfate) on the catalytic performa nce of the pr...In this paper,the CuO-CeO_(2) catalyst was prepared by a direct solvothermal method.The effects of different copper salt precursors(copper nitrate,copper acetate,copper sulfate) on the catalytic performa nce of the prepared catalyst fo r CO oxidation were investigated.The physical and chemical properties of the prepared catalysts were characterized by X-ray diffraction(XRD),Raman spectroscopy,N_(2)physical adsorption,inductively coupled plasma-atomic emission spectrometry(ICP-AES),X-ray photoelectron spectroscopy(XPS),temperature-programmed desorption analysis of CO(CO-TPD),in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTs),and temperature-programmed reduction with H_(2)(H_(2)-TPR).The results show that the CuO-CeO_(2)catalyst prepared with copper acetate as precursor(CC-A) exhibits the best catalytic activity for CO oxidation at low temperatures,with T50and T90values of 62 and 78℃ respectively,which is mainly attributed to its large specific surface area,pore volume,CO adsorption capacity,and large amount and strong reactivity of surface oxygen.However,the CuO-CeO_(2) catalyst prepared with copper nitrate as precursor(CC-N) displays better stability and resistance to water or CO_(2) poisoning than CC-A.展开更多
In this work,various Co_(3)O_(4)-ZSM-5 catalysts were prepared by the microwave hydrothermal method(MH-Co_(3)O_(4)@ZSM-5),dynamic hydrothermal method(DH-Co_(3)O_(4)@ZSM-5),and conventio nal hydrothermal method(CH-Co_(...In this work,various Co_(3)O_(4)-ZSM-5 catalysts were prepared by the microwave hydrothermal method(MH-Co_(3)O_(4)@ZSM-5),dynamic hydrothermal method(DH-Co_(3)O_(4)@ZSM-5),and conventio nal hydrothermal method(CH-Co_(3)O_(4)/ZSM-5).Their catalytic oxidation of dichloromethane(DCM)was analyzed.Detailed characterizations such as X-ray diffractometer(XRD),scanning microscopy(SEM),X-ray photoelectron spectroscopy(XPS),Brunauer-Emmett-Teller(BET),H2 temperature-programmed reduction(H2-TPR),temperature-programmed desorption of O_(2)(O_(2)-TPD),temperature-programmed desorption of NH_(3)(NH_(3)-TPD),diffuse reflectance infrared Fourier-transform spectra with NH_(3)molecules(NH_(3)-DRIFT),and temperature-programmed surface reaction(TPSR)were performed.Results showed that with the assistance of microwave,MH-Co_(3)O_(4)@ZSM-5 formed a uniform core-shell structure,while the other two samples did not.MH-Co_(3)O_(4)@ZSM-5 possessed rich surface adsorbed oxygen species,higher ratio of Co^(3+)/Co^(2+),strong acidity,high reducibility,and oxygen mobility among the three Co_(3)O_(4)-ZSM-5 catalysts,which was beneficial for the improvement of DCM oxidation.In the oxidation of dichloromethane,MH-Co_(3)O_(4)@ZSM-5 presented the best activity and mineralization,which was consistent with the characterizations results.Meanwhile,according to the TPSR test,HCl or Cl_(2)removal from the catalyst surface was also promoted in MH-Co_(3)O_(4)@ZSM-5 by their abundant Bronsted acid sites and the promotion of Deacon reaction by Co_(3)O_(4)or the synergistic effect of Co_(3)O_(4)and ZSM-5.According to the results of in situ DRIFT studies,a possible reaction pathway of DCM oxidation was proposed over the MH-Co_(3)O_(4)@ZSM-5 catalysts.展开更多
The oil oxidation characteristics of the whole temperature regions from 30 ℃ to 600 ℃ during oil reservoir air injection were revealed by experiments. The whole oil oxidation temperature regions were divided into fo...The oil oxidation characteristics of the whole temperature regions from 30 ℃ to 600 ℃ during oil reservoir air injection were revealed by experiments. The whole oil oxidation temperature regions were divided into four different parts: dissolving and inflation region, low temperature oxidation region, medium temperature oxidation region and high temperature oxidation region. The reaction mechanisms of different regions were explained. Based on the oil oxidation characteristics and filed tests results, light oil reservoirs air injection development methods were divided into two types: oxygen-reducing air flooding and air flooding;heavy oil reservoirs air injection in-situ combustion development methods were divided into two types: medium temperature in-situ combustion and high temperature in-situ combustion. When the reservoir temperature is lower than 120 ℃, oxygen-reducing air flooding should be used for light oil reservoir development. When the reservoir temperature is higher than 120 ℃, air flooding method should be used for light oil reservoir development. For a normal heavy oil reservoir, when the combustion front temperature is lower than 400 ℃, the development method is medium temperature in-situ combustion. For a heavy oil reservoir with high oil resin and asphalting contents, when the combustion front temperature is higher than 450 ℃, the development method at this condition is high temperature in-situ combustion. Ten years field tests of air injection carried out by PetroChina proved that air has advantages in technical, economical and gas source aspects compared with other gas agents for oilfield gas injection development. Air injection development can be used in low/super-low permeability light oil reservoirs, medium and high permeability light oil reservoirs and heavy oil reservoirs. Air is a very promising gas flooding agent.展开更多
Walnuts are rich in a variety of nutritional components.However,due to their high content of unsaturated fatty acids(UFAs),the quality of walnuts tends to decline during storage,which adversely affects the development...Walnuts are rich in a variety of nutritional components.However,due to their high content of unsaturated fatty acids(UFAs),the quality of walnuts tends to decline during storage,which adversely affects the development of the walnut industry.This study was aimed to investigate the impacts of temperature and packaging methods on the storage quality and oxidative stability of walnuts.The Wen 185 walnut variety was selected,and the physical-chemical and nutritional indexes of walnuts stored for 42 weeks under different temperatures(18℃,4℃,and room temperature)and packaging methods(vacuum light-exposed,vacuum light-proof,vacuum-ra-diation light-exposed,vacuum-radiation light-proof,nitrogen-filled light-exposed,nitrogen-filled light-proof)were measured.The results showed that low temperatures,especially18℃,in combination with vacuum lightproof packaging,could effectively suppress the increase in oxidative stability indicators such as acid value(AV)and peroxide value(PV),and maintain high retention rates of nutritional indicators like tocopherol and phytosterol.This study has elucidated that low temperatures and appropriate packaging methods play the crucial roles in maintaining the quality and oxidative stability of walnuts during storage.It has provided comprehensive and valuable data support and theoretical basis for the scientific storage of walnuts,contributing to the devel-opment of the walnut industry and the guarantee of product quality.展开更多
The use of metal oxides has been extensively documented in the literature and applied in a variety of contexts,including but not limited to energy storage,chemical sensors,and biomedical applications.One of the most s...The use of metal oxides has been extensively documented in the literature and applied in a variety of contexts,including but not limited to energy storage,chemical sensors,and biomedical applications.One of the most significant applications of metal oxides is heterogeneous catalysis,which represents a pivotal technology in industrial production on a global scale.Catalysts serve as the primary enabling agents for chemical reactions,and among the plethora of catalysts,metal oxides including magnesium oxide(MgO),ceria(CeO_(2))and titania(TiO_(2)),have been identified to be particularly effective in catalyzing a variety of reactions[1].Theoretical calculations based on density functional theory(DFT)and a multitude of other quantum chemistry methods have proven invaluable in elucidating the mechanisms of metal-oxide-catalyzed reactions,thereby facilitating the design of high-performance catalysts[2].展开更多
Pd/Al_(2)O_(3)was pretreated by CO,H_(2)and NaBH_(4)reduction,respectively.The reduced catalysts were tested for o-xylene oxidation and characterized by power X-ray diffraction(XRD),transmission electron microscopy (T...Pd/Al_(2)O_(3)was pretreated by CO,H_(2)and NaBH_(4)reduction,respectively.The reduced catalysts were tested for o-xylene oxidation and characterized by power X-ray diffraction(XRD),transmission electron microscopy (TEM),X-ray photoelectron spectroscopy (XPS) and temperature-programmed decomposition of palladium hydride (TPDH).The characterizations indicate the pretreatments lead to distinct Pd particle sizes and amount of surface activated oxygen species,which are responsible for the catalytic performance.Compared with H_(2)and NaBH_(4)reduction methods,CO reduction shows a strong interaction between Pd and Al_(2)O_(3)with smaller Pd particle size and more surface activated oxygen.It exhibited excellent catalytic performance,complete oxidation of 50 ppmV o-xylene at 85℃with a WHSV of 60,000 mL/(g·hr).展开更多
基金supported by the State Key Laboratory of Urban Water Resource and Environment,Harbin Institute of Technology (No. 2022TS10)the Taishan Industrial Experts Programthe Natural Science Foundation of Shandong Province of China (No. ZR2023ME212).
文摘Wet flue gas desulfurization(WFGD)could effectively reduce sulfur dioxide emission.However,magnesium sulfite(MgSO_(3)),a by-product of desulfurization,was easy to result in secondary pollution.In this study,the solid catalyst Co-Bent(bentonite supported cobalt)was prepared by blending method for MgSO_(3) oxidation with bentonite as the carrier and cobalt as the active component.At the calcination temperature of 550℃ and the Co loading level of 3 wt.%,the catalyst showed excellent catalytic performance for the oxidation of high concentration MgSO_(3) slurry,and the oxidation rate of MgSO_(3) was 0.13 mol/(L·h).The research indicated that the active component was uniformly distributed within porous structure of the catalyst as Co_(3)O_(4),which facilitated the oxidation of SO_(3)^(2-) catalyzed by Co_(3)O_(4).Kinetic researches indicated the oxidation rate of MgSO_(3) was influenced by the catalyst dosage,the reaction temperature,the solution pH,the airflow rate,and the SO_(3)^(2-) concentration.Additionally,after recycling experiments,the regenerated catalyst retained its high catalytic performance for the MgSO_(3) oxidation.The reaction mechanism for the catalytic oxidation of MgSO_(3) by Co-Bent catalyst was also proposed.The generation of active free radicals(OH·,SO_(4)^(-)·,SO_(3)^(-)·,SO_(5)^(-)·)accelerated the MgSO_(3) oxidation.These results provide theoretical support for the treatment of MgSO_(3) and the development of durable catalyst.
基金Project supported by the National Natural Science Foundation of China(21203254)Natural Science Foundation of Hubei Province(2015CFA138)+1 种基金Natural Science Foundation of Liaoning Province(201602681)Shenyang Municipal Science and Technology Planning Projects(17-76-1-00)
文摘Perovskite oxides LaCoO3 prepared by templating,co-precipitation and sol-gel method with different complexants were systematically characterized and its catalytic performances for CO oxidation were investigated.The samples were characterized by X-ray diffraction,thermogravimetry analysis and differential scanning calorimetry,N2 physisorption,transmission electron microscopy,temperature program reduction of hydrogen,temperature program desorption of oxygen and X-ray photoelectron spectroscopy measurement,results of which show that the properties of LaCoO3,such as surface morphology,surface area,surface compositions,redox capability,oxygen vacancy,as well as the calcination temperature and formation mechanism,depend intimately on the preparation method.Catalytic tests indicate that the sample prepared by carbon templating method shows the best activity for CO oxidation,with full CO conversion obtained at 135℃.In particular,the catalyst can be activated and significant increase of activity can be obtained with the increase of reaction time.The cyclic and longterm stability of catalysts were discussed and compared.
文摘Influence of three different preparation methods, i.e. impregnation, coprecipitation, and inverse coprecipitation, on the preferential oxidation of CO in excess hydrogen （PROX） over CuO-CeO2 catalysts has been investigated and CuO-CeO2 catalysts are characterized using BET, XPS, XRD, UV Raman, and TPR techniques. The results show that the catalysts prepared by coprecipitation have smaller particle sizes, well-dispersed CuOx species, more oxygen vacancies, and are more active in the PROX than those prepared by the other methods. However. the inverse coprecipitation depresses the catalytic performance of CuO-CeO2 catalysts and causes the growth of CuO-CeO2 because of different pH value in the precipitation process.
基金supported by the National Natural Science Foundation of China (21263015,21567016 and 21503106)the Education Department Foundation of Jiangxi Province (KJLD14005 and GJJ150016)the Natural Science Foundation of Jiangxi Province (20142BAB213013 and 20151BBE50006),which are greatly acknowledged by the authors~~
文摘A series of SnO2‐based catalysts modified by Mn, Zr, Ti and Pb oxides with a Sn/M （M=Mn, Zr, Ti and Pb） molar ratio of 9/1 were prepared by a co‐precipitation method and used for CH4 and CO oxidation. The Mn3＋, Zr4＋, Ti4＋and Pb4＋cations are incorporated into the lattice of tetragonal rutile SnO2 to form a solid solution structure. As a consequence, the surface area and thermal stability of the catalysts are improved. Moreover, the oxygen species of the modified catalysts become easier to be reduced. Therefore, the oxidation activity over the catalysts was improved, except for the one modified by Pb oxide. Manganese oxide demonstrates the best promotional effects for SnO2. Using an X‐ray diffraction extrapolation method, the lattice capacity of SnO2 for Mn2O3 was 0.135 g Mn2O3/g SnO2, which indicates that to form stable solid solution, only 21%Sn4＋cations in the lattice can be maximally replaced by Mn3＋. If the amount of Mn3＋cations is over the capacity, Mn2O3 will be formed, which is not favorable for the activity of the catalysts. The Sn rich samples with only Sn‐Mn solid solution phase show higher activity than the ones with excess Mn2O3 species.
基金supported by the Nationals Key Research and Development Program of China (No.2017YFC0210600)the National Natural Science Foundation of China (No.51978644)。
文摘Based on the demand of sintering/pelleting flue gas ultra-low emission,a semi-dry method using a spray dryer absorber (SDA) combined with O3 oxidation was proposed for simultaneous removal of SO2 and NO.Effects of O3 injection site,O3/NO molar ratio,and spray tower temperature on the removal efficiencies were investigated.It was revealed that both desulfurization and denitrification efficiencies could reach to 85%under the conditions of setting O3 injection site inside of tower,O3/NO molar ratio 1.8,spray tower temperature 85°C,Ca/(S+2N) molar ratio 2.5 and slurry flow rate 300 m L/hr.CaSO3/Ca(OH)2 mixture slurry was used as absorbent to simulate operating conditions in iron and steel industry.The result shows that the addition of CaSO3 weakens both removal efficiencies.In addition,the reaction mechanism of simultaneous removal of SO2 and NO using SDA combined with O3 oxidation was proposed.
基金supported financially by the China Scholarship Council(No.201706340114).
文摘Facile green oxidation methods are always desired to functionalize carbon nanotubes(CNTs)in the production of advanced CNT/epoxy composites.In the present work,an optimized H2O2/H2O/O3 oxidation method was developed,and performances of the H2O2/H2O/O3 oxidized CNT in epoxy matrix were tested and compared with that of the H2O/O3 oxidized CNT and the most commonly used concentrated HNO3 oxidized CNT.The physical and chemical characteristics of the obtained oxidized CNTs were systematically characterized via transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS)and Raman.Mechanical performances of the obtained composites were explored by tensile tests,impact tests,dynamic mechanical analysis(DMA)and fracture toughness tests.It was found that the H2O2/H2O/O3 oxidized CNT exhibited all-around overwhelming advantages over the concentrated HNO3 oxidized CNT on reinforcing the epoxy matrix,while the H2O/O3 oxidized CNT only improved the material strength.Reinforcing mechanisms for the different methods oxidized CNTs were studied and compared.The optimized H2O2/H2O/O3 oxidation method makes scaled production possible,avoids environment pollutions,and holds great potentials to replace the most commonly used concentrated HNO3 oxidation method to oxidize CNT during the preparation of the advanced CNT/epoxy composite.
基金supported by the National Key Research and Development Program of China(No.2017YFC0210600)the National Natural Science Foundation of China(No.51978644)。
文摘With the vigorous development of China's iron and steel industry and the introduction of ultra-low emission policies,the emission of pollutants such as SO_(2)and NO x has received unprecedented attention.Considering the increase of the proportion of semi-dry desulfurization technology in the desulfurization process,several semi-dry desulphurization technologies such as flue gas circulating fluidized bed(CFB),dense flow absorber(DFA)and spray drying absorption(SDA)are briefly summarized.Moreover,a method for simultaneous treatment of SO_(2)and NOx in sintering/pelletizing flue gas by O_(3)oxidation combined with semidry method is introduced.Meantime,the effects of key parameters such as O_(3)/NO molar ratio,Ca SO_(3),SO_(2),reaction temperature,Ca/(S+2 N)molar ratio,droplet size and approach to adiabatic saturation temperature(AAST)on denitrification and desulfurization are analyzed.Furthermore,the reaction mechanism of denitrification and desulfurization is further elucidated.Finally,the advantages and development prospects of the new technology are proposed.
基金supported by the National Nature Science Foundation of China (Project No.20576023)the Natural Science Foundation of Guangdong Province (Project No.06025660).
文摘The Cu-Zr-Ce-O catalysts prepared using the coprecipitation method exhibited better catalytic performance for CO selective oxidation. The Cu-Zr-Ce-O catalysts pretreated with different methods were studied by CO-TPR and XPS techniques. The results showed that the Cu-Zr-Ce-O catalyst pretreated with oxygen exhibited the best catalytic performance and had the widest operating temperature window, with CO conversion above 99% from 160 to 200 ℃. The O2 pretreatment caused an enrichment of the oxygen storaged on the Cu active species and promoted the conversion of adsorbed oxygen into surface lattice oxygen. It also improved the amount of Cu＋/Cu^2＋ ionic pair, and then facilitated the formation of CuO active species on the catalyst for selective CO oxidation.
基金the Shanxi Provin-cial Youth Science and Technology Research Fund (No.2008021009-2) for the financial support to this project
文摘The removal of hydrogen sulfide from gas plays an important role in rational utilization of resources and environ- mental protection. In this paper, the process of hydrogen sulfide removal by wet oxidation method in a rotating packed bed was investigated in a scale for treating 10 000 Nm3/h of gas. On the basis of studying the influence of the species and con- centration of alkali source, the liquid/gas volume ratio, the high gravity factor, and the hydrogen sulfide content in feed gas on the desulfurization effect, the suitable technological conditions were obtained. The hydrogen sulfide removal efficiency could reach 98.0% under these conditions. The results of continuous operation of process facilities showed that the high gravity method has many merits including higher desulfurization rate, good stability in operation, lower liquid/gas volume ratio, greater operation elasticity, and apparent energy saving effects.
基金Project supported by Shanghai Science and Technology Commission(11nm0501600)
文摘A novel and convenient hydrolysis and oxidation method was first used in preparation of carbon contained Y2O3 phosphor powders. The alloy was hydrolyzed in deionized water and the obtained Y（OH）3 powders were heat treated in air atmosphere. The final products - Y2O3 powders were micron clusters which were aggregated by hundreds of nanoparticles with the size of about 5 nm. The chemical composition, structural and morphological features of the samples were characterized by means of X-ray powder diffraction （XRD） analysis, transmission electron microscopy （TEM）, Fourier-transform infrared （FT-IR） spectra, X-ray photoelectron spectra （XPS） and carbon sulfur analyzer. The obtained powders showed good bluish-white photoluminescence （PL） emissions （ranging from 430 to 600 nm, peaking at 468 nm and 578 nm） under the xenon light excitation. The luminescent mechanism was ascribed to the carbon impurities in the Y2O3 host.
基金The work was supported by the National Basic Research Program of China (973 Program, No. 2004CB719504)
文摘The CuO-CeO2 catalyst prepared by chelating method has a superior catalytic performance for the preferential oxidation of CO in rich hydrogen, compared with the CuO-CeO2 catalyst prepared by coprecipitation method. The CO conversions over these catalysts, at 120 ℃ and 120000 ml/（g-h） in the absence of CO2 and H2O, are 99.6% and 88.6%, respectively, and the selectivity of O2 over these catalysts is very close （i.e. 51.3% and 55.8%, respectively）. The influence of certain factors such as hydrogen concentration, carbon monoxide concentration, H2O, O2/CO ratios, and space velocity on the catalytic performance of CuO-CeO2 catalyst prepared by chelating method is also studied. The results show that the addition of hydrogen and H2O has a negative effect on the catalytic performance of CuO-CeO2 catalyst, however, the variation of space velocity and the O2/CO ratio causes a comparatively slight influence.
基金Funded by Scientific and Technological Innovation Project of Carbon Emission Peak and Carbon Neutrality of Jiangsu Province(No.BE2022028-4)。
文摘We adopted the solution impregnation route with aluminum dihydrogen phosphate solution as liquid medium for effective surface modification on graphite substrate.The mass ratio of graphite to Al(H_(2)PO_(4))_(3) changed from 0.5:1 to 4:1,and the impregnation time changed from 1 to 7 h.The typical composite phase change thermal storage materials doped with the as-treated graphite were fabricated using form-stable technique.To investigate the oxidation and anti-oxidation behavior of the impregnated graphite at high temperatures,the samples were put into a muffle furnace for a cyclic heat test.Based on SEM,EDS,DSC techniques,analyses on the impregnated technique suggested an optimized processing conditions of a 3 h impregnation time with the ratio of graphite:Al(H_(2)PO_(4))_(3) as 1:3 for graphite impregnation treatment.Further investigations on high-temperature phase change heat storage materials doped by the treated graphite suggested excellent oxidation resistance and thermal cycling performance.
基金Project supported by the National Natural Science Foundation of China (Nos. 90505015 and10702035)
文摘High-temperature oxidation is an important property to evaluate thermal protection materials. However, since oxidation is a complex process involving microstructure evolution, its quantitative analysis has always been a challenge. In this work, a phase field method （PFM） based on the thermodynamics theory is developed to simulate the oxidation behavior and oxidation induced growth stress. It involves microstructure evolution and solves the problem of quantitatively computational analysis for the oxidation behavior and growth stress. Employing this method, the diffusion process, oxidation performance, and stress evolution axe predicted for Fe-Cr-A1-Y alloys. The numerical results agree well with the experimental data. The linear relationship between the maximum growth stress and the environment oxygen concentration is found. PFM provides a powerful tool to investigate high-temperature oxidation in complex environments.
文摘The influence of different cooking and smoking methods (boiling, frying, frying + boiling, hot and cold smoking) on oxidation and fatty acid composition of catfish (Arius maculatus) commercialized on the Wouri river coast was evaluated including commonly used analytical indexes (peroxide and acid values)and physical analysis by Fourier transform infrared (FTIR) spectroscopy. The mean moisture, protein, ash and fat contents of raw fish were 75.88 ± 0.55;64.24 ± 0.14;10.98 ± 0.31 and 23.02 ± 0.88 respectively. All these treatments provoke the modification of the quality indexes. Lipid deterioration, thermolysis and lipid oxidation occurred throughout the treatment. Peroxide value decreased for all cooked and smoked catfish, while free fatty acids of smoked sample increased. The FTIR applied to evaluate lipid oxidation in extracted lipid clearly provided a better picture of the oxidation progress and led to a similar conclusion with chemical analysis. Boiled, bleaching hot and bleaching cold smoking were found to be the suitable treatment methods for catfish because they gave it a high nutritive value compared to other smoking methods.
基金Project supported by the National Natural Science Foundation of China (21273150)。
文摘In this paper,the CuO-CeO_(2) catalyst was prepared by a direct solvothermal method.The effects of different copper salt precursors(copper nitrate,copper acetate,copper sulfate) on the catalytic performa nce of the prepared catalyst fo r CO oxidation were investigated.The physical and chemical properties of the prepared catalysts were characterized by X-ray diffraction(XRD),Raman spectroscopy,N_(2)physical adsorption,inductively coupled plasma-atomic emission spectrometry(ICP-AES),X-ray photoelectron spectroscopy(XPS),temperature-programmed desorption analysis of CO(CO-TPD),in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTs),and temperature-programmed reduction with H_(2)(H_(2)-TPR).The results show that the CuO-CeO_(2)catalyst prepared with copper acetate as precursor(CC-A) exhibits the best catalytic activity for CO oxidation at low temperatures,with T50and T90values of 62 and 78℃ respectively,which is mainly attributed to its large specific surface area,pore volume,CO adsorption capacity,and large amount and strong reactivity of surface oxygen.However,the CuO-CeO_(2) catalyst prepared with copper nitrate as precursor(CC-N) displays better stability and resistance to water or CO_(2) poisoning than CC-A.
基金financially supported by the National Natural Science Foundation of China(No.51708492)National Key Research and Development Plan of China(No.2016YFC0204700)+1 种基金Zhejiang Provincial"151"Talents Programthe Program for Zhejiang Leading Team of S&T Innovation(No.2013TD07)。
文摘In this work,various Co_(3)O_(4)-ZSM-5 catalysts were prepared by the microwave hydrothermal method(MH-Co_(3)O_(4)@ZSM-5),dynamic hydrothermal method(DH-Co_(3)O_(4)@ZSM-5),and conventio nal hydrothermal method(CH-Co_(3)O_(4)/ZSM-5).Their catalytic oxidation of dichloromethane(DCM)was analyzed.Detailed characterizations such as X-ray diffractometer(XRD),scanning microscopy(SEM),X-ray photoelectron spectroscopy(XPS),Brunauer-Emmett-Teller(BET),H2 temperature-programmed reduction(H2-TPR),temperature-programmed desorption of O_(2)(O_(2)-TPD),temperature-programmed desorption of NH_(3)(NH_(3)-TPD),diffuse reflectance infrared Fourier-transform spectra with NH_(3)molecules(NH_(3)-DRIFT),and temperature-programmed surface reaction(TPSR)were performed.Results showed that with the assistance of microwave,MH-Co_(3)O_(4)@ZSM-5 formed a uniform core-shell structure,while the other two samples did not.MH-Co_(3)O_(4)@ZSM-5 possessed rich surface adsorbed oxygen species,higher ratio of Co^(3+)/Co^(2+),strong acidity,high reducibility,and oxygen mobility among the three Co_(3)O_(4)-ZSM-5 catalysts,which was beneficial for the improvement of DCM oxidation.In the oxidation of dichloromethane,MH-Co_(3)O_(4)@ZSM-5 presented the best activity and mineralization,which was consistent with the characterizations results.Meanwhile,according to the TPSR test,HCl or Cl_(2)removal from the catalyst surface was also promoted in MH-Co_(3)O_(4)@ZSM-5 by their abundant Bronsted acid sites and the promotion of Deacon reaction by Co_(3)O_(4)or the synergistic effect of Co_(3)O_(4)and ZSM-5.According to the results of in situ DRIFT studies,a possible reaction pathway of DCM oxidation was proposed over the MH-Co_(3)O_(4)@ZSM-5 catalysts.
文摘The oil oxidation characteristics of the whole temperature regions from 30 ℃ to 600 ℃ during oil reservoir air injection were revealed by experiments. The whole oil oxidation temperature regions were divided into four different parts: dissolving and inflation region, low temperature oxidation region, medium temperature oxidation region and high temperature oxidation region. The reaction mechanisms of different regions were explained. Based on the oil oxidation characteristics and filed tests results, light oil reservoirs air injection development methods were divided into two types: oxygen-reducing air flooding and air flooding;heavy oil reservoirs air injection in-situ combustion development methods were divided into two types: medium temperature in-situ combustion and high temperature in-situ combustion. When the reservoir temperature is lower than 120 ℃, oxygen-reducing air flooding should be used for light oil reservoir development. When the reservoir temperature is higher than 120 ℃, air flooding method should be used for light oil reservoir development. For a normal heavy oil reservoir, when the combustion front temperature is lower than 400 ℃, the development method is medium temperature in-situ combustion. For a heavy oil reservoir with high oil resin and asphalting contents, when the combustion front temperature is higher than 450 ℃, the development method at this condition is high temperature in-situ combustion. Ten years field tests of air injection carried out by PetroChina proved that air has advantages in technical, economical and gas source aspects compared with other gas agents for oilfield gas injection development. Air injection development can be used in low/super-low permeability light oil reservoirs, medium and high permeability light oil reservoirs and heavy oil reservoirs. Air is a very promising gas flooding agent.
基金Key Technology Research and Development Program in Autonomous Region(2022A02009)Agricultural Science and Technology Innovation Project of Chinese Academy of Agricultural Sciences(CAAS-ASTIP-2021-OCRI).
文摘Walnuts are rich in a variety of nutritional components.However,due to their high content of unsaturated fatty acids(UFAs),the quality of walnuts tends to decline during storage,which adversely affects the development of the walnut industry.This study was aimed to investigate the impacts of temperature and packaging methods on the storage quality and oxidative stability of walnuts.The Wen 185 walnut variety was selected,and the physical-chemical and nutritional indexes of walnuts stored for 42 weeks under different temperatures(18℃,4℃,and room temperature)and packaging methods(vacuum light-exposed,vacuum light-proof,vacuum-ra-diation light-exposed,vacuum-radiation light-proof,nitrogen-filled light-exposed,nitrogen-filled light-proof)were measured.The results showed that low temperatures,especially18℃,in combination with vacuum lightproof packaging,could effectively suppress the increase in oxidative stability indicators such as acid value(AV)and peroxide value(PV),and maintain high retention rates of nutritional indicators like tocopherol and phytosterol.This study has elucidated that low temperatures and appropriate packaging methods play the crucial roles in maintaining the quality and oxidative stability of walnuts during storage.It has provided comprehensive and valuable data support and theoretical basis for the scientific storage of walnuts,contributing to the devel-opment of the walnut industry and the guarantee of product quality.
基金financial support from the National Key R&D Program of China(2021YFB3500700)the National Natural Science Foundation of China(22473042,22003016,and 92145302).
文摘The use of metal oxides has been extensively documented in the literature and applied in a variety of contexts,including but not limited to energy storage,chemical sensors,and biomedical applications.One of the most significant applications of metal oxides is heterogeneous catalysis,which represents a pivotal technology in industrial production on a global scale.Catalysts serve as the primary enabling agents for chemical reactions,and among the plethora of catalysts,metal oxides including magnesium oxide(MgO),ceria(CeO_(2))and titania(TiO_(2)),have been identified to be particularly effective in catalyzing a variety of reactions[1].Theoretical calculations based on density functional theory(DFT)and a multitude of other quantum chemistry methods have proven invaluable in elucidating the mechanisms of metal-oxide-catalyzed reactions,thereby facilitating the design of high-performance catalysts[2].
基金supported by the National Natural Science Foundation of China (Nos. 21936005 and 21806011)。
文摘Pd/Al_(2)O_(3)was pretreated by CO,H_(2)and NaBH_(4)reduction,respectively.The reduced catalysts were tested for o-xylene oxidation and characterized by power X-ray diffraction(XRD),transmission electron microscopy (TEM),X-ray photoelectron spectroscopy (XPS) and temperature-programmed decomposition of palladium hydride (TPDH).The characterizations indicate the pretreatments lead to distinct Pd particle sizes and amount of surface activated oxygen species,which are responsible for the catalytic performance.Compared with H_(2)and NaBH_(4)reduction methods,CO reduction shows a strong interaction between Pd and Al_(2)O_(3)with smaller Pd particle size and more surface activated oxygen.It exhibited excellent catalytic performance,complete oxidation of 50 ppmV o-xylene at 85℃with a WHSV of 60,000 mL/(g·hr).
