The pressurized combustion experiments of bituminous coal and lignite under air and O2/CO2 atmospheres were conducted to study the influences of pressure and atmosphere on combustion and the CO, NO, SO2 release proces...The pressurized combustion experiments of bituminous coal and lignite under air and O2/CO2 atmospheres were conducted to study the influences of pressure and atmosphere on combustion and the CO, NO, SO2 release process. Two indices, the maximum concentration and the total emission, were applied to quantitatively evaluate the influence of several different operating parameters such as pressure, atmosphere and temperature on the formation of NO and SO2 during coal combustion in the fluidized bed. The experimental results show that the releasing profiles of CO, NO and SO2 during coal combustion under a pressurized oxy- fuel atmosphere are similar to those under a pressurized air atmosphere, and the curves of measured gas components are all unimodal. Under the oxy-fuel condition, pressure increasing from 0.1 to 0.7 MPa can cause the inhibition of NO and SO2 emission. The elevation of temperature can lead to an increase in the maximum concentration and the total production of NO and SO2, and the increase under atmospheric pressure is higher than that under high pressure.展开更多
Engineering the morphology of the support is effective in tuning the redox properties of active metals for efficient catalytic methane combustion via tailoring the metal-support interaction.Herein,uniform Ir nanoparti...Engineering the morphology of the support is effective in tuning the redox properties of active metals for efficient catalytic methane combustion via tailoring the metal-support interaction.Herein,uniform Ir nanoparticles supported on anatase TiO_(2)with different morphologies predominantly exposing{100},{101},and{001}planes were synthesized and tested for methane combustion.The CH_(4) catalytic activity shows a remarkable TiO_(2)-facet-dependent effect and follows the order of Ir/TiO_(2)-{100}>Ir/TiO_(2)-{101}>>Ir/TiO_(2)-{001}.Detailed characterizations and DFT calculations reveal that compared with Ir-TiO_(2)-{101}and Ir-TiO_(2)-{001}interfaces,the superior Ir-TiO_(2)-{100}interface facilitates the generation of electron-rich Ir species through more profound charge transfer from TiO_(2)-{100}to Ir atoms.The electron-rich Ir structure,featuring abundant defect oxygen vacancies,significantly enhances the redox properties of active Ir species and reduces the activation energy for breaking the initial C-H bond in CH_(4),resulting in the superior catalytic activity for methane combustion.These findings deepen fundamental insights into the TiO_(2)-facet-dependent reactivity of different Ir/TiO_(2)nanomaterials in methane oxidation and pave the way for designing efficient Ir-based methane oxidation catalysts.展开更多
The thermogravimetric analyzer and horizontal tube furnace are used to study the effects of operation parameters such as temperature, fuel type, and oxygen concentration on the combustion and NO emission characteristi...The thermogravimetric analyzer and horizontal tube furnace are used to study the effects of operation parameters such as temperature, fuel type, and oxygen concentration on the combustion and NO emission characteristics of the rice husk, rice straw, and peanut shell in the O2/CO2 atmosphere. The results show that the combustion performances of volatile matter and fixed carbon of the three biomasses increase with the increase in the 02 content. The mean NO emission increases sharply when the reaction temperature increases from 700 to 800℃. However, it increases slightly when the temperature exceeds 800 ℃. Meanwhile, the mean NO emission and nitrogen conversion decrease with the increase in the nitrogen content in biomass. The mean NO emission changes little with different oxygen concentrations, and the NO emissions of the three biomasses are all lower than the requirement for the minimum NO emission. Increasing the oxygen concentration favors the biomass combustion in the O2/CO2 atmosphere, and oxygen concentration has little effect on the NO emission.展开更多
A 20 wt% Ni/bentonite catalyst was prepared by a solution combustion synthesis (SCS), which exhibited higher activity for the CO_2methanation than that of an impregnation method (IPM), and the catalyst prepared by SCS...A 20 wt% Ni/bentonite catalyst was prepared by a solution combustion synthesis (SCS), which exhibited higher activity for the CO_2methanation than that of an impregnation method (IPM), and the catalyst prepared by SCS showed a CO_2 conversion of 85% and a CH4selectivity of 100% at 300 °C, atmospheric pressure, and 3600 ml·(g cat)-1·h-1, and the catalyst exhibited stable within a 110-h reaction. The results showed higher me- tallic Ni dispersion, smaller Ni particle size, larger specific surface area and lower reduction temperature in the Ni/ bentonite prepared by SCS than that of IPM. And the Ni/bentonite prepared by the SCS moderated the interaction between NiO and bentonite.展开更多
A series of Ni/ZrO_2 catalysts were synthesized by urea combustion method for CO_2 methanation.The effects of zirconium precursors and urea dosage on the structure and catalytic performance of the catalysts were teste...A series of Ni/ZrO_2 catalysts were synthesized by urea combustion method for CO_2 methanation.The effects of zirconium precursors and urea dosage on the structure and catalytic performance of the catalysts were tested.Results showed that the Ni/ZrO_2–O catalyst derived from zirconium oxynitrate hydrate exhibited better catalytic activity than the Ni/ZrO_2 catalyst because of its higher Ni dispersion and smaller Ni particle size.In addition,the urea dosage significantly influenced the low-temperature activity of the catalysts by affecting the metal–support interaction,Ni dispersion,and Ni particle size.The Ni/ZrO_2–O-0.4 catalyst with a urea-to-nitrate molar ratio of 0.4 exhibited the best catalytic activity owing to its moderate metal–support interaction,highest Ni dispersion,and smallest Ni particle size,achieving 69.2% CO_2 conversion and 100% CH_4 selectivity at 300℃,0.1 MPa,and a weight hour space velocity(WHSV)of 50,000 mL/(g·h).Moreover,the urea combustion method can lead to the entire phase transformation from monoclinic ZrO_2 to tetragonal ZrO_2 accompanied by the incorporation of oxygen vacancies in the ZrO_2 lattice.This phenomenon can also be related to the high catalytic activity of the as-prepared catalysts.展开更多
At present monoethanolamine(MEA) remains as the standard industrial solvent for CO_2 capture processes. But due to the degradation and high energy consumption problems of MEA, new efficient solvents should be found. I...At present monoethanolamine(MEA) remains as the standard industrial solvent for CO_2 capture processes. But due to the degradation and high energy consumption problems of MEA, new efficient solvents should be found. In the present work, the absorption and regeneration performance of a hybrid solvent MEA-methanol was studied and compared to the aqueous solutions of monoethanolamine(MEA), diethanolamine(DEA) and triethanolamine(TEA) in a bubbling reactor. Also the performance of MEA-methanol solutions(including the absorption performance, regeneration performance,cyclic absorption performance, density and viscosity) was studied with different MEA concentrations. A pilot-plant CO_2 capture test bed was used to study the potential of MEA-methanol to replace aqueous MEA in industrial use. The results showed that the initial absorption rate of MEA-methanol solvent is the fastest compared with other solvents. The 30% MEA-methanol had a faster mass transfer coefficient, a higher CO_2 absorption efficiency and a lower regeneration energy consumption than aqueous MEA. And through the study of the reaction heat of CO_2 into MEA-methanol and aqueous MEA,it can be concluded that the desorption heat of rich MEA-methanol is only about 30% of rich aqueous MEA solvent in the regeneration process which showed that 30% MEA-methanol solvent is a promising candidate for CO_2 capture.展开更多
The temperature dependence on the reaction of desulfurization reagent CaCO3 and SO2 in O2/CO2 coal combustion was investigated by thcrmogravimetric analysis, X-ray diffraction measurement and pore structure analysis. ...The temperature dependence on the reaction of desulfurization reagent CaCO3 and SO2 in O2/CO2 coal combustion was investigated by thcrmogravimetric analysis, X-ray diffraction measurement and pore structure analysis. The results show that the conversion of the reaction of CaCO3 and SO2 in air is higher at 500-1 100 ℃ and lower at 1 200 ℃ compared with that in O2/CO2 atmosphere. The conversion can be increased by increasing the concentration of SO2, which causes the inhibition of CaSO4 decomposition and shifting of the reaction equilibrium toward the products. XRD analysis of the product shows that the reaction mechanism of CaCO3 and SO2 differs with temperature in O2/CO2 atmosphere, i.e. CaCO3 directly reacts with SO2 at 500 ℃ and CaO from CaCO3 decomposition reacts with SO2 at 1 000 ℃. The pore analysis of the products indicates that the maximum specific surface area of the products accounts for the highest conversion at 1 100 ℃ in O2/CO2 atmosphere. The results reveal that the effect of the atmosphere on the conversion is temperature dependence.展开更多
Benzylamine(BZA) has been identified as a promising candidate for CO_2 capture process; however the evaluation of BZA in the packed column was very few. Thus, in this work, the absorption and regeneration performance ...Benzylamine(BZA) has been identified as a promising candidate for CO_2 capture process; however the evaluation of BZA in the packed column was very few. Thus, in this work, the absorption and regeneration performance of unblended BZA solvent as well as a series of amine concentrations and ratios in the formulations were studied using a semibatch bubbling reactor. And due to the formation of ivory-white precipitates in solvents containing higher BZA ratios, a 4:1 molar ratio of MEA/BZA mixed solvent was used to study its performance in a pilot-scale test bed. The results showed that a higher BZA ratio in the MEA/BZA mixed solvent resulted in a faster absorption rate, a higher mass transfer and heat transfer rate and a better cyclic performance, but the mass transfer rate of BZA decreased more quickly than MEA with the increase of CO_2 loading of the solvents. In addition, at high CO_2 loading in the MEA/ BZA mixed solvent with a molar ratio of 4:1, the ivory-white precipitates were generated which could cause blockage of the packing in the absorber, the stripper and the liquid pipelines.展开更多
Long-term manure application has the potential to alleviate soil acidification, and increase carbon sequestration and nutrient availability, thus improving cropland fertility. However, the mechanisms behind greenhouse...Long-term manure application has the potential to alleviate soil acidification, and increase carbon sequestration and nutrient availability, thus improving cropland fertility. However, the mechanisms behind greenhouse gas N_(2)O emissions from acidic soil mediated by long-term manure application remain poorly understood. Herein, we investigated N_(2)O emission and its linkage with gross N mineralization and nitrification rates, as well as nitrifying and denitrifying microbes in an acidic upland soil subjected to 36-year fertilization treatments, including an unfertilized control(CK), inorganic fertilizer(F), 2× rate of inorganic fertilizer(2F), manure(M), and the combination of inorganic fertilizer and manure(FM) treatments. Compared to the CK treatment(1.34 μg N kg^(-1) d^(-1)), fertilization strongly increased N_(2)O emissions by 34-fold on average, with more pronounced increases in the manure-amendment(10.6-169 μg N kg^(-1) d^(-1)) than those in the inorganic fertilizer treatments(3.26-5.51 μg N kg^(-1) d^(-1)). The manure amendment-stimulated N_(2)O emissions were highly associated with increased soil pH, mean weight diameter of soil aggregates, substrate availability(e.g., particulate organic carbon, NO_(3)^(-)and available phosphorus), gross N mineralization rates, denitrifier abundances and the(nirK+nirS)/nosZ ratio. These findings suggest that the increased N_(2)O emissions primarily resulted from alleviated acidification, increased substrate availability and improved soil structure, thus enhancing microbial N mineralization and favoring N_(2)O^(-)producing denitrifiers over N_(2)O consumers. Moreover, ammonia-oxidizing bacteria(AOB) rather than ammonia-oxidizing archaea(AOA) positively correlated with soil NO_(3)^(-)concentration and N_(2)O emissions, indicating that nitrification indirectly contributed to N_(2)O production by supplying NO_(3)^(-)for denitrification. Collectively, manure amendment potentially stimulates N_(2)O emissions, primarily resulting from alleviated soil acidification and increased substrate availability, thus enhancing N mineralization and denitrifier-mediated N_(2)O production. Our findings suggest that consideration should be given to the greenhouse gas budgets of agricultural ecosystems when applying manure for managing the pH and fertility of acidic soils.展开更多
SO2 release and removal were studied under both the air and oxy-fuel combustion conditions using an anthracite coal from the Jincheng mine in China on a bench-scale fluidized bed combustor （FBC）. Special attention w...SO2 release and removal were studied under both the air and oxy-fuel combustion conditions using an anthracite coal from the Jincheng mine in China on a bench-scale fluidized bed combustor （FBC）. Special attention was paid to the effects of the combustion atmosphere, 02 concentration, bed temperature, and limestone addition. The released amount of SO2 was clearly higher under 30% 02/70% CO2 than that of the air atmosphere. As the O2 concentration in O2/CO2 mixture increased from 21% to 40%, the released amount of SO2 increased significantly, but then it decreased when the 02 concentration increased up to 50%. The bed temperature from 860 to 920 ℃ has no obvious influence on the the SO2 release but shows a strong influence on the desulfurization with limestone in both oxy-fuel and air conditions. The maximum SO2 removal efficiency appears to be at 880 to 900 ℃ for both the air and oxy-fuel combustion conditions.展开更多
Ni-Y2O3 nanocomposite powder with uniform distribution of fine oxide particles in the metal matrix was successfully fabricated via solution combustion process followed by hydrogen reduction. The combustion behavior wa...Ni-Y2O3 nanocomposite powder with uniform distribution of fine oxide particles in the metal matrix was successfully fabricated via solution combustion process followed by hydrogen reduction. The combustion behavior was investigated by DTA-TG analysis. The influence of urea to nickel nitrate（U/Ni） ratio on the combustion behavior and morphology evolution of the combusted powder was investigated. The morphological characteristics and phase transformation of the combusted powder and the reduced powder were characterized by FESEM, TEM and XRD. The HRTEM image of Ni-Y2O3 nanocomposite powder indicated that Y2O3 particles with average particle size of about 10 nm dispersed uniformly in the nickel matrix.展开更多
The non-grinding long afterglow material SrAl2O4：Eu^2＋ , Dy^3＋ was prepared by combustion method in home mierowave oven direetly, after dispersant, frother, eomburent, and mineralizer were added into the reacting s...The non-grinding long afterglow material SrAl2O4：Eu^2＋ , Dy^3＋ was prepared by combustion method in home mierowave oven direetly, after dispersant, frother, eomburent, and mineralizer were added into the reacting system. XRD analysis showed that the powders were nearly pure SrAl2O4 phase with few other phases, and the size of the grain was 41.1 nm. Fluoreseenee speetrum results indieated that there were 2 exeitation peaks loeated at 345 and 400 nm, and the emission peak loeated at 516 nm, afterglow lasted up to 30 min or more. The mierowave eombustion method has advantages of less time, low temperature and no grinding process, and the material made by the method has good luminescent property.展开更多
Activity and stability of 1%Pd-0.2%Pt/Al2O3 and 1%Pd-0.2%Pt/0.6%Ce/Al2O3 catalysts prepared by impregnation method for catalytic combustion of methane in air were investigated. The catalysts before and after reaction ...Activity and stability of 1%Pd-0.2%Pt/Al2O3 and 1%Pd-0.2%Pt/0.6%Ce/Al2O3 catalysts prepared by impregnation method for catalytic combustion of methane in air were investigated. The catalysts before and after reaction were characterized by BET, CO chemisorption, XRD and XPS techniques. Results showed that the presence of Ce significantly increased the activity and thermal stability of the Pd-Pt/Al2O3 catalyst towards methane combustion, which could be attributed to more highly-dispersed active PdO particles over the Pd-Pt/Ce/Al2O3 catalyst surface as well as the retarded sintering of PdO and the maintained oxidized state of surface Pd during the combustion process in the presence of Ce.展开更多
Cubic and monoclinic Gd2O3:Eu3+ phosphors in the range of nano-scale and submicron-scale were prepared by a modified solution combustion method.Coexistence of cubic and monoclinic phases was found in the highest lumin...Cubic and monoclinic Gd2O3:Eu3+ phosphors in the range of nano-scale and submicron-scale were prepared by a modified solution combustion method.Coexistence of cubic and monoclinic phases was found in the highest luminescent sample synthesized at 600 oC.In relation to commercial sample,the relative luminescence intensity was 49.8%.The shape of emission spectrum of the sample thus changed and the charge-transfer-state band of excitation spectrum slightly shift toward higher energies.With increasing the anneal...展开更多
Galvanic deposition method was used to prepare the Pd/Ni-Al2O3-GD catalyst for the combustion of methane under lean conditions. The new catalyst and compared catalysts （Pd/Al2O3-IW, Pd-Ni/Al2O3-IW, Pd/Ni-Al2O3-IW） p...Galvanic deposition method was used to prepare the Pd/Ni-Al2O3-GD catalyst for the combustion of methane under lean conditions. The new catalyst and compared catalysts （Pd/Al2O3-IW, Pd-Ni/Al2O3-IW, Pd/Ni-Al2O3-IW） prepared by incipient wetness impregnation were characterized by N2-physisorption, XRD and TEM to clarify particle size and size distribution of palladium species. Combined O2-TPD and XPS results with the catalytic data, it shows that the surface palladium species with low valence exhibits better combustion performance due to their stronger interaction with support. The results indicate that the galvanic deposition method is an effective route to prepare efficient catalyst for methane combustion, and it also provides useful information for improving the present commercial catalyst.展开更多
Chemical looping combustion （CLC） of carbonaceous compounds has been proposed, in the past decade, as an efficient method for CO2 capture without cost of extra energy penalties. The technique involves the use of a m...Chemical looping combustion （CLC） of carbonaceous compounds has been proposed, in the past decade, as an efficient method for CO2 capture without cost of extra energy penalties. The technique involves the use of a metal oxide as an oxygen carrier that transfers oxygen from combustion air to fuels. The combustion is carried out in a two-step process： in the fuel reactor, the fuel is oxidized by a metal oxide, and in the air reactor, the reduced metal is oxidized back to the original phase. The use of iron oxide as an oxygen carrier has been investigated in this article. Particles composed of 80 wt% Fe2O3, together with Al2O3 as binder, have been prepared by impregnation methods. X-ray diffraction （XRD） analysis reveals that Fe2O3 does not interact with the Al2O3 binder after multi-cycles. The reactivity of the oxygen carrier particles has been studied in twenty-cycle reduction-oxidation tests in a thermal gravimetrical analysis （TGA） reactor. The components in the outlet gas have been analyzed. It has been observed that about 85% of CH4 converted to CO2 and H2O during most of the reduction periods. The oxygen carrier has kept quite a high reactivity in the twenty-cycle reactions. In the first twenty reaction cycles, the reaction rates became slightly higher with the number of cyclic reactions increasing, which was confirmed by the scanning electron microscopy （SEM） test results. The SEM analysis revealed that the pore size inside the particle had been enlarged by the thermal stress during the reaction, which was favorable for diffusion of the gaseous reactants into the particles. The experimental results suggested that the Fe2O3/Al2O3 oxygen carrier was a promising candidate for a CLC system.展开更多
In this paper,MCM-41 was synthesized by a soft template technique and MCM-41 supported CuO-CeO2 nano-sized catalysts with different Cu/Ce molar ratios were prepared by a deposition-precipitation method.N2 adsorption,H...In this paper,MCM-41 was synthesized by a soft template technique and MCM-41 supported CuO-CeO2 nano-sized catalysts with different Cu/Ce molar ratios were prepared by a deposition-precipitation method.N2 adsorption,HRTEM-EDS,H2-TPR,XPS characterization,as well as catalytic activity and durability tests for the catalytic combustion of chlorobenzene(CB)were conducted to explore the relationship between the structure and catalytic performance of the catalysts.It is revealed that cuCe(6:1)/MCM-41 has the highest activity and can completely catalyze the degradation of CB at 260℃.The reasons for the high activity of the catalysts are as follows:MCM-41,a type of mesoporous material which has large pore size and large specific surface area,is suitable as a catalyst carrier.The average diameter of nano-sized CuO and CeO2 particles is about 3-5 nm and adding CeO2 improves the dispersion of active component CuO,which are highly and evenly dispersed on the surface of MCM-41.Characterization results also explain why MCM-41 supported CuO-CeO2 with appropriate proportion can highly enhance the catalytic activity.The reason is that CeO2 acting as an oxygen-rich material can improve the mobility of oxygen species through continuous redox between Ce4^+and Ce3^+,and improve the catalytic performance of CuO for CB combustion.Besides,CuCe(6:1)/MCM-41 also displays good durability for CB combustion,both in the humid condition and in the presence of benzene,making it a promising catalytic material for the elimination of chlorinated VOCs.展开更多
Blue-green luminescent BaAl2O4：Eu2＋,Dy3＋ phosphor powders were synthesized via combustion synthesis method assisted by microwave irradiation in air. The phosphors were characterized by X-ray diffraction （XRD）, sc...Blue-green luminescent BaAl2O4：Eu2＋,Dy3＋ phosphor powders were synthesized via combustion synthesis method assisted by microwave irradiation in air. The phosphors were characterized by X-ray diffraction （XRD）, scanning electron microscopy （SEM） and fluorescence spectrophotometer. The XRD results revealed that when the concentration of urea was over 3 times higher than theoretical quantities, a BaAl2O4 single hexagonal phase was obtained. The SEM results revealed that the surface of the BaAl2O4：Eu2＋,Dy3＋ powder samples showed lots of voids and pores. The BaAl2O4：Eu2＋,Dy3＋ phosphors exhibited a broad emission band of main peak at 496 nm and a shoulder peak at 426 nm under excitation of 337 nm. The BaAl2O4：Eu2＋,Dy3＋ phosphors at the Eu2＋ concentration of 1 mol.% showed the strongest luminescent intensity. Long afterglow phosphorescence was observed in the dark with naked eyes after the removal of the excitation source.展开更多
A series of Ceo.sFeo.30Zr0.20O2 catalysts were prepared by different methods （co-precipitations method, citric acid sol-gel method, impregnation method, physical mixed method, and hydrotherrnal method） and character...A series of Ceo.sFeo.30Zr0.20O2 catalysts were prepared by different methods （co-precipitations method, citric acid sol-gel method, impregnation method, physical mixed method, and hydrotherrnal method） and characterized by X-ray diffraction （XRD）, Raman spectroscopy, Brunauer-Emmett-Teller （BET） and H2-TPR measurements. Potential of the catalysts in the soot oxidation was evaluated in a temperature-programmed oxidation （TPO） apparatus. The results showed that all the Fe3＋ and Zr4＋ were incor- porated into ceria lattice to form a pure Ce-Fe-Zr-O solid solution for the co-precipitation sample, but two kinds of Fe phases ex- isted in the Ce-Fe-Zr-O catalysts prepared by other methods： Fe3＋ incorporated into CeO2 lattice and dispersed Fe2O3 clusters. The free Fe2O3 clusters could improve the activity of catalysts for soot oxidation comparing with the pure Ce-Fe-Zr-O solid solution owing to the synergetic effect between free Fe2O3 and surface oxygen vacancies. In addition, the activity of catalysts strongly relied on the surface reducibility of free Fe2O3 particles. Holding both abundant free Fe2O3 particles and high oxygen vacancy concentration, the hydrothermal Ce0.5Fe0.3Zr0.202 catalyst presented the lowest Ti （251℃, ignition temperature of soot oxidation） and Tm （310 ℃, maximum oxidation rate temperature） for soot combustion （with tight-contact between soot and catalysts） among the five samples. Even after aging at 800 ℃ for 10 h, the Ti and Tm were still relatively low, at 273 and 361 ℃, respectively, indicating high catalytic stability.展开更多
Chemical looping combustion （CLC） of coal has gained increasing attention as a novel combustion technology for its advantages in CO2 capture. Sulfur evolution from coal causes great harm from either the CLC operatio...Chemical looping combustion （CLC） of coal has gained increasing attention as a novel combustion technology for its advantages in CO2 capture. Sulfur evolution from coal causes great harm from either the CLC operational or environmental perspective. In this research, a combined MnFe2O4 oxygen carrier （OC） was synthesized and its reaction with a typical Chinese high sulfur coal, Liuzhi （LZ） bituminous coal, was performed in a thermogravimetric analyzer （TGA）-Fourier transform infrared （FT-IR） spectrometer. Evolution of sulfur species during reaction of LZ coal with MnFeaO40C was systematically investigated through experimental means combined with thermodynamic simulation. TGA-FTIR analysis of the LZ reaction with MnFe2O4 indicated MnFe2O4 exhibited the desired superior reactivity compared to the single reference oxides Mn304 or Fe203, and SO2 produced was mainly related to oxidization of H2S by MnFe2O4. Experimental analysis of the LZ coal reaction with MnFe2O4, including X-ray diffraction and X-ray photoelectron spectroscopy analysis, verified that the main reduced counterparts of MnFe2O4 were Fe304 and MnO, in good agreement with the related thermodynamic simulation. The obtained MnO was beneficial to stabilize the reduced MnFe2O4 and avoid serious sintering, although the oxygen in MnO was not fully utilized. Meanwhile, most sulfur present in LZ coal was converted to solid MnS during LZ reaction with MnFe2O4, which was further oxidized to MnSO4. Finally, the formation of both MnS and such manganese silicates as Mn2SiO4 and MnSiO3 should be addressed to ensure the full regeneration of the reduced MnFe2O4.展开更多
基金The National Natural Science Foundation of China(No.51206023)the National Key Basic Research Program of China(973 Program)(No.2011CB707301-3)the Fundamental Research Funds for the Central Universities
文摘The pressurized combustion experiments of bituminous coal and lignite under air and O2/CO2 atmospheres were conducted to study the influences of pressure and atmosphere on combustion and the CO, NO, SO2 release process. Two indices, the maximum concentration and the total emission, were applied to quantitatively evaluate the influence of several different operating parameters such as pressure, atmosphere and temperature on the formation of NO and SO2 during coal combustion in the fluidized bed. The experimental results show that the releasing profiles of CO, NO and SO2 during coal combustion under a pressurized oxy- fuel atmosphere are similar to those under a pressurized air atmosphere, and the curves of measured gas components are all unimodal. Under the oxy-fuel condition, pressure increasing from 0.1 to 0.7 MPa can cause the inhibition of NO and SO2 emission. The elevation of temperature can lead to an increase in the maximum concentration and the total production of NO and SO2, and the increase under atmospheric pressure is higher than that under high pressure.
文摘Engineering the morphology of the support is effective in tuning the redox properties of active metals for efficient catalytic methane combustion via tailoring the metal-support interaction.Herein,uniform Ir nanoparticles supported on anatase TiO_(2)with different morphologies predominantly exposing{100},{101},and{001}planes were synthesized and tested for methane combustion.The CH_(4) catalytic activity shows a remarkable TiO_(2)-facet-dependent effect and follows the order of Ir/TiO_(2)-{100}>Ir/TiO_(2)-{101}>>Ir/TiO_(2)-{001}.Detailed characterizations and DFT calculations reveal that compared with Ir-TiO_(2)-{101}and Ir-TiO_(2)-{001}interfaces,the superior Ir-TiO_(2)-{100}interface facilitates the generation of electron-rich Ir species through more profound charge transfer from TiO_(2)-{100}to Ir atoms.The electron-rich Ir structure,featuring abundant defect oxygen vacancies,significantly enhances the redox properties of active Ir species and reduces the activation energy for breaking the initial C-H bond in CH_(4),resulting in the superior catalytic activity for methane combustion.These findings deepen fundamental insights into the TiO_(2)-facet-dependent reactivity of different Ir/TiO_(2)nanomaterials in methane oxidation and pave the way for designing efficient Ir-based methane oxidation catalysts.
基金The Natural Science Foundation of Anhui Province(No.1508085ME73)the Open Foundation of Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education(No.201406)
文摘The thermogravimetric analyzer and horizontal tube furnace are used to study the effects of operation parameters such as temperature, fuel type, and oxygen concentration on the combustion and NO emission characteristics of the rice husk, rice straw, and peanut shell in the O2/CO2 atmosphere. The results show that the combustion performances of volatile matter and fixed carbon of the three biomasses increase with the increase in the 02 content. The mean NO emission increases sharply when the reaction temperature increases from 700 to 800℃. However, it increases slightly when the temperature exceeds 800 ℃. Meanwhile, the mean NO emission and nitrogen conversion decrease with the increase in the nitrogen content in biomass. The mean NO emission changes little with different oxygen concentrations, and the NO emissions of the three biomasses are all lower than the requirement for the minimum NO emission. Increasing the oxygen concentration favors the biomass combustion in the O2/CO2 atmosphere, and oxygen concentration has little effect on the NO emission.
基金Supported by the National Natural Science Foundation of China(21566005)the Natural Science Foundation of Guangxi Province(2016GXNSFFA380015)
文摘A 20 wt% Ni/bentonite catalyst was prepared by a solution combustion synthesis (SCS), which exhibited higher activity for the CO_2methanation than that of an impregnation method (IPM), and the catalyst prepared by SCS showed a CO_2 conversion of 85% and a CH4selectivity of 100% at 300 °C, atmospheric pressure, and 3600 ml·(g cat)-1·h-1, and the catalyst exhibited stable within a 110-h reaction. The results showed higher me- tallic Ni dispersion, smaller Ni particle size, larger specific surface area and lower reduction temperature in the Ni/ bentonite prepared by SCS than that of IPM. And the Ni/bentonite prepared by the SCS moderated the interaction between NiO and bentonite.
文摘A series of Ni/ZrO_2 catalysts were synthesized by urea combustion method for CO_2 methanation.The effects of zirconium precursors and urea dosage on the structure and catalytic performance of the catalysts were tested.Results showed that the Ni/ZrO_2–O catalyst derived from zirconium oxynitrate hydrate exhibited better catalytic activity than the Ni/ZrO_2 catalyst because of its higher Ni dispersion and smaller Ni particle size.In addition,the urea dosage significantly influenced the low-temperature activity of the catalysts by affecting the metal–support interaction,Ni dispersion,and Ni particle size.The Ni/ZrO_2–O-0.4 catalyst with a urea-to-nitrate molar ratio of 0.4 exhibited the best catalytic activity owing to its moderate metal–support interaction,highest Ni dispersion,and smallest Ni particle size,achieving 69.2% CO_2 conversion and 100% CH_4 selectivity at 300℃,0.1 MPa,and a weight hour space velocity(WHSV)of 50,000 mL/(g·h).Moreover,the urea combustion method can lead to the entire phase transformation from monoclinic ZrO_2 to tetragonal ZrO_2 accompanied by the incorporation of oxygen vacancies in the ZrO_2 lattice.This phenomenon can also be related to the high catalytic activity of the as-prepared catalysts.
基金supported by the Sinopec Ningbo Engineering Co., Ltd.(No.l4850000-14-ZC0609-0003, H8XY-0032)
文摘At present monoethanolamine(MEA) remains as the standard industrial solvent for CO_2 capture processes. But due to the degradation and high energy consumption problems of MEA, new efficient solvents should be found. In the present work, the absorption and regeneration performance of a hybrid solvent MEA-methanol was studied and compared to the aqueous solutions of monoethanolamine(MEA), diethanolamine(DEA) and triethanolamine(TEA) in a bubbling reactor. Also the performance of MEA-methanol solutions(including the absorption performance, regeneration performance,cyclic absorption performance, density and viscosity) was studied with different MEA concentrations. A pilot-plant CO_2 capture test bed was used to study the potential of MEA-methanol to replace aqueous MEA in industrial use. The results showed that the initial absorption rate of MEA-methanol solvent is the fastest compared with other solvents. The 30% MEA-methanol had a faster mass transfer coefficient, a higher CO_2 absorption efficiency and a lower regeneration energy consumption than aqueous MEA. And through the study of the reaction heat of CO_2 into MEA-methanol and aqueous MEA,it can be concluded that the desorption heat of rich MEA-methanol is only about 30% of rich aqueous MEA solvent in the regeneration process which showed that 30% MEA-methanol solvent is a promising candidate for CO_2 capture.
基金Project(50525619) supported by the National Natural Science Foundation of ChinaProject(306012) supported by the Key Foundation of Ministry of Education of China
文摘The temperature dependence on the reaction of desulfurization reagent CaCO3 and SO2 in O2/CO2 coal combustion was investigated by thcrmogravimetric analysis, X-ray diffraction measurement and pore structure analysis. The results show that the conversion of the reaction of CaCO3 and SO2 in air is higher at 500-1 100 ℃ and lower at 1 200 ℃ compared with that in O2/CO2 atmosphere. The conversion can be increased by increasing the concentration of SO2, which causes the inhibition of CaSO4 decomposition and shifting of the reaction equilibrium toward the products. XRD analysis of the product shows that the reaction mechanism of CaCO3 and SO2 differs with temperature in O2/CO2 atmosphere, i.e. CaCO3 directly reacts with SO2 at 500 ℃ and CaO from CaCO3 decomposition reacts with SO2 at 1 000 ℃. The pore analysis of the products indicates that the maximum specific surface area of the products accounts for the highest conversion at 1 100 ℃ in O2/CO2 atmosphere. The results reveal that the effect of the atmosphere on the conversion is temperature dependence.
基金supported by the Sinopec Ningbo Engineering Co. Ltd. (No.l4850000-14-ZC0609-0003,H8XY-0032)
文摘Benzylamine(BZA) has been identified as a promising candidate for CO_2 capture process; however the evaluation of BZA in the packed column was very few. Thus, in this work, the absorption and regeneration performance of unblended BZA solvent as well as a series of amine concentrations and ratios in the formulations were studied using a semibatch bubbling reactor. And due to the formation of ivory-white precipitates in solvents containing higher BZA ratios, a 4:1 molar ratio of MEA/BZA mixed solvent was used to study its performance in a pilot-scale test bed. The results showed that a higher BZA ratio in the MEA/BZA mixed solvent resulted in a faster absorption rate, a higher mass transfer and heat transfer rate and a better cyclic performance, but the mass transfer rate of BZA decreased more quickly than MEA with the increase of CO_2 loading of the solvents. In addition, at high CO_2 loading in the MEA/ BZA mixed solvent with a molar ratio of 4:1, the ivory-white precipitates were generated which could cause blockage of the packing in the absorber, the stripper and the liquid pipelines.
基金financially supported by the National Science & Technology Fundamental Resources Investigation Project of China (2021FY100501)the Youth Innovation of Chinese Academy of Agricultural Sciences (Y2023QC16)。
文摘Long-term manure application has the potential to alleviate soil acidification, and increase carbon sequestration and nutrient availability, thus improving cropland fertility. However, the mechanisms behind greenhouse gas N_(2)O emissions from acidic soil mediated by long-term manure application remain poorly understood. Herein, we investigated N_(2)O emission and its linkage with gross N mineralization and nitrification rates, as well as nitrifying and denitrifying microbes in an acidic upland soil subjected to 36-year fertilization treatments, including an unfertilized control(CK), inorganic fertilizer(F), 2× rate of inorganic fertilizer(2F), manure(M), and the combination of inorganic fertilizer and manure(FM) treatments. Compared to the CK treatment(1.34 μg N kg^(-1) d^(-1)), fertilization strongly increased N_(2)O emissions by 34-fold on average, with more pronounced increases in the manure-amendment(10.6-169 μg N kg^(-1) d^(-1)) than those in the inorganic fertilizer treatments(3.26-5.51 μg N kg^(-1) d^(-1)). The manure amendment-stimulated N_(2)O emissions were highly associated with increased soil pH, mean weight diameter of soil aggregates, substrate availability(e.g., particulate organic carbon, NO_(3)^(-)and available phosphorus), gross N mineralization rates, denitrifier abundances and the(nirK+nirS)/nosZ ratio. These findings suggest that the increased N_(2)O emissions primarily resulted from alleviated acidification, increased substrate availability and improved soil structure, thus enhancing microbial N mineralization and favoring N_(2)O^(-)producing denitrifiers over N_(2)O consumers. Moreover, ammonia-oxidizing bacteria(AOB) rather than ammonia-oxidizing archaea(AOA) positively correlated with soil NO_(3)^(-)concentration and N_(2)O emissions, indicating that nitrification indirectly contributed to N_(2)O production by supplying NO_(3)^(-)for denitrification. Collectively, manure amendment potentially stimulates N_(2)O emissions, primarily resulting from alleviated soil acidification and increased substrate availability, thus enhancing N mineralization and denitrifier-mediated N_(2)O production. Our findings suggest that consideration should be given to the greenhouse gas budgets of agricultural ecosystems when applying manure for managing the pH and fertility of acidic soils.
基金The National Natural Science Foundation for Young Scholars of China(No.51106038)the National Key Technology R&D Program of China during the 12th Five-Year Plan Period(No.2012BAA02B01-04)
文摘SO2 release and removal were studied under both the air and oxy-fuel combustion conditions using an anthracite coal from the Jincheng mine in China on a bench-scale fluidized bed combustor （FBC）. Special attention was paid to the effects of the combustion atmosphere, 02 concentration, bed temperature, and limestone addition. The released amount of SO2 was clearly higher under 30% 02/70% CO2 than that of the air atmosphere. As the O2 concentration in O2/CO2 mixture increased from 21% to 40%, the released amount of SO2 increased significantly, but then it decreased when the 02 concentration increased up to 50%. The bed temperature from 860 to 920 ℃ has no obvious influence on the the SO2 release but shows a strong influence on the desulfurization with limestone in both oxy-fuel and air conditions. The maximum SO2 removal efficiency appears to be at 880 to 900 ℃ for both the air and oxy-fuel combustion conditions.
基金Project(2132046)supported by the Beijing Natural Science Foundation,ChinaProject(51104007)supported by the National Natural Science Foundation of China
文摘Ni-Y2O3 nanocomposite powder with uniform distribution of fine oxide particles in the metal matrix was successfully fabricated via solution combustion process followed by hydrogen reduction. The combustion behavior was investigated by DTA-TG analysis. The influence of urea to nickel nitrate（U/Ni） ratio on the combustion behavior and morphology evolution of the combusted powder was investigated. The morphological characteristics and phase transformation of the combusted powder and the reduced powder were characterized by FESEM, TEM and XRD. The HRTEM image of Ni-Y2O3 nanocomposite powder indicated that Y2O3 particles with average particle size of about 10 nm dispersed uniformly in the nickel matrix.
基金Project supported by the National Natural Science Foundation of China (20476002)
文摘The non-grinding long afterglow material SrAl2O4：Eu^2＋ , Dy^3＋ was prepared by combustion method in home mierowave oven direetly, after dispersant, frother, eomburent, and mineralizer were added into the reacting system. XRD analysis showed that the powders were nearly pure SrAl2O4 phase with few other phases, and the size of the grain was 41.1 nm. Fluoreseenee speetrum results indieated that there were 2 exeitation peaks loeated at 345 and 400 nm, and the emission peak loeated at 516 nm, afterglow lasted up to 30 min or more. The mierowave eombustion method has advantages of less time, low temperature and no grinding process, and the material made by the method has good luminescent property.
基金supported by the National High Technology Research and Development Program (863) of China (No.2010AA064904)
文摘Activity and stability of 1%Pd-0.2%Pt/Al2O3 and 1%Pd-0.2%Pt/0.6%Ce/Al2O3 catalysts prepared by impregnation method for catalytic combustion of methane in air were investigated. The catalysts before and after reaction were characterized by BET, CO chemisorption, XRD and XPS techniques. Results showed that the presence of Ce significantly increased the activity and thermal stability of the Pd-Pt/Al2O3 catalyst towards methane combustion, which could be attributed to more highly-dispersed active PdO particles over the Pd-Pt/Ce/Al2O3 catalyst surface as well as the retarded sintering of PdO and the maintained oxidized state of surface Pd during the combustion process in the presence of Ce.
基金supported by the Ministry of Science and Technology of China (2006CB601104)the Foundation of International Joint Research of Beijing (2007N08)+1 种基金Natural Science Foundation of Jiangxi Province (2009GQC0042)Foundation of Jiangxi Educational Committee (GJJ10153)
文摘Cubic and monoclinic Gd2O3:Eu3+ phosphors in the range of nano-scale and submicron-scale were prepared by a modified solution combustion method.Coexistence of cubic and monoclinic phases was found in the highest luminescent sample synthesized at 600 oC.In relation to commercial sample,the relative luminescence intensity was 49.8%.The shape of emission spectrum of the sample thus changed and the charge-transfer-state band of excitation spectrum slightly shift toward higher energies.With increasing the anneal...
基金supported by the National Natural Science Foundation of China (21273221)the National High Technology Research and Development Program of China (863 Program, 2011AA03A406)
文摘Galvanic deposition method was used to prepare the Pd/Ni-Al2O3-GD catalyst for the combustion of methane under lean conditions. The new catalyst and compared catalysts （Pd/Al2O3-IW, Pd-Ni/Al2O3-IW, Pd/Ni-Al2O3-IW） prepared by incipient wetness impregnation were characterized by N2-physisorption, XRD and TEM to clarify particle size and size distribution of palladium species. Combined O2-TPD and XPS results with the catalytic data, it shows that the surface palladium species with low valence exhibits better combustion performance due to their stronger interaction with support. The results indicate that the galvanic deposition method is an effective route to prepare efficient catalyst for methane combustion, and it also provides useful information for improving the present commercial catalyst.
基金Supported by the National Natural Science Foundation of China (No.50574046 and 50164002, )Natural Science Foun-dation of Yunnan Province (No. 2004E0012Q).
文摘Chemical looping combustion （CLC） of carbonaceous compounds has been proposed, in the past decade, as an efficient method for CO2 capture without cost of extra energy penalties. The technique involves the use of a metal oxide as an oxygen carrier that transfers oxygen from combustion air to fuels. The combustion is carried out in a two-step process： in the fuel reactor, the fuel is oxidized by a metal oxide, and in the air reactor, the reduced metal is oxidized back to the original phase. The use of iron oxide as an oxygen carrier has been investigated in this article. Particles composed of 80 wt% Fe2O3, together with Al2O3 as binder, have been prepared by impregnation methods. X-ray diffraction （XRD） analysis reveals that Fe2O3 does not interact with the Al2O3 binder after multi-cycles. The reactivity of the oxygen carrier particles has been studied in twenty-cycle reduction-oxidation tests in a thermal gravimetrical analysis （TGA） reactor. The components in the outlet gas have been analyzed. It has been observed that about 85% of CH4 converted to CO2 and H2O during most of the reduction periods. The oxygen carrier has kept quite a high reactivity in the twenty-cycle reactions. In the first twenty reaction cycles, the reaction rates became slightly higher with the number of cyclic reactions increasing, which was confirmed by the scanning electron microscopy （SEM） test results. The SEM analysis revealed that the pore size inside the particle had been enlarged by the thermal stress during the reaction, which was favorable for diffusion of the gaseous reactants into the particles. The experimental results suggested that the Fe2O3/Al2O3 oxygen carrier was a promising candidate for a CLC system.
基金Project supported by the National Natural Science Foundation of China(21577094)Zhejiang Public Welfare Technology Research Project(LGG19B070003)the Foundation of Science and Technology of Shaoxing City(2018C10019)。
文摘In this paper,MCM-41 was synthesized by a soft template technique and MCM-41 supported CuO-CeO2 nano-sized catalysts with different Cu/Ce molar ratios were prepared by a deposition-precipitation method.N2 adsorption,HRTEM-EDS,H2-TPR,XPS characterization,as well as catalytic activity and durability tests for the catalytic combustion of chlorobenzene(CB)were conducted to explore the relationship between the structure and catalytic performance of the catalysts.It is revealed that cuCe(6:1)/MCM-41 has the highest activity and can completely catalyze the degradation of CB at 260℃.The reasons for the high activity of the catalysts are as follows:MCM-41,a type of mesoporous material which has large pore size and large specific surface area,is suitable as a catalyst carrier.The average diameter of nano-sized CuO and CeO2 particles is about 3-5 nm and adding CeO2 improves the dispersion of active component CuO,which are highly and evenly dispersed on the surface of MCM-41.Characterization results also explain why MCM-41 supported CuO-CeO2 with appropriate proportion can highly enhance the catalytic activity.The reason is that CeO2 acting as an oxygen-rich material can improve the mobility of oxygen species through continuous redox between Ce4^+and Ce3^+,and improve the catalytic performance of CuO for CB combustion.Besides,CuCe(6:1)/MCM-41 also displays good durability for CB combustion,both in the humid condition and in the presence of benzene,making it a promising catalytic material for the elimination of chlorinated VOCs.
基金supported by the National Natural Science Foundation of China (60477034)
文摘Blue-green luminescent BaAl2O4：Eu2＋,Dy3＋ phosphor powders were synthesized via combustion synthesis method assisted by microwave irradiation in air. The phosphors were characterized by X-ray diffraction （XRD）, scanning electron microscopy （SEM） and fluorescence spectrophotometer. The XRD results revealed that when the concentration of urea was over 3 times higher than theoretical quantities, a BaAl2O4 single hexagonal phase was obtained. The SEM results revealed that the surface of the BaAl2O4：Eu2＋,Dy3＋ powder samples showed lots of voids and pores. The BaAl2O4：Eu2＋,Dy3＋ phosphors exhibited a broad emission band of main peak at 496 nm and a shoulder peak at 426 nm under excitation of 337 nm. The BaAl2O4：Eu2＋,Dy3＋ phosphors at the Eu2＋ concentration of 1 mol.% showed the strongest luminescent intensity. Long afterglow phosphorescence was observed in the dark with naked eyes after the removal of the excitation source.
基金Project supported by National Natural Science Foundation of China(51374004,51204083,51174105,51104074)Natural Science Foundation of Yunnan Province(2010ZC018)
文摘A series of Ceo.sFeo.30Zr0.20O2 catalysts were prepared by different methods （co-precipitations method, citric acid sol-gel method, impregnation method, physical mixed method, and hydrotherrnal method） and characterized by X-ray diffraction （XRD）, Raman spectroscopy, Brunauer-Emmett-Teller （BET） and H2-TPR measurements. Potential of the catalysts in the soot oxidation was evaluated in a temperature-programmed oxidation （TPO） apparatus. The results showed that all the Fe3＋ and Zr4＋ were incor- porated into ceria lattice to form a pure Ce-Fe-Zr-O solid solution for the co-precipitation sample, but two kinds of Fe phases ex- isted in the Ce-Fe-Zr-O catalysts prepared by other methods： Fe3＋ incorporated into CeO2 lattice and dispersed Fe2O3 clusters. The free Fe2O3 clusters could improve the activity of catalysts for soot oxidation comparing with the pure Ce-Fe-Zr-O solid solution owing to the synergetic effect between free Fe2O3 and surface oxygen vacancies. In addition, the activity of catalysts strongly relied on the surface reducibility of free Fe2O3 particles. Holding both abundant free Fe2O3 particles and high oxygen vacancy concentration, the hydrothermal Ce0.5Fe0.3Zr0.202 catalyst presented the lowest Ti （251℃, ignition temperature of soot oxidation） and Tm （310 ℃, maximum oxidation rate temperature） for soot combustion （with tight-contact between soot and catalysts） among the five samples. Even after aging at 800 ℃ for 10 h, the Ti and Tm were still relatively low, at 273 and 361 ℃, respectively, indicating high catalytic stability.
基金supported by the National Natural Science Foundation of China(No.51276210,50906030,50936001)the financial grant of North China University of Water Conservancy and Electric Power(No.201012)the National Basic Research Program(973)of China(No.2011CB707301)
文摘Chemical looping combustion （CLC） of coal has gained increasing attention as a novel combustion technology for its advantages in CO2 capture. Sulfur evolution from coal causes great harm from either the CLC operational or environmental perspective. In this research, a combined MnFe2O4 oxygen carrier （OC） was synthesized and its reaction with a typical Chinese high sulfur coal, Liuzhi （LZ） bituminous coal, was performed in a thermogravimetric analyzer （TGA）-Fourier transform infrared （FT-IR） spectrometer. Evolution of sulfur species during reaction of LZ coal with MnFeaO40C was systematically investigated through experimental means combined with thermodynamic simulation. TGA-FTIR analysis of the LZ reaction with MnFe2O4 indicated MnFe2O4 exhibited the desired superior reactivity compared to the single reference oxides Mn304 or Fe203, and SO2 produced was mainly related to oxidization of H2S by MnFe2O4. Experimental analysis of the LZ coal reaction with MnFe2O4, including X-ray diffraction and X-ray photoelectron spectroscopy analysis, verified that the main reduced counterparts of MnFe2O4 were Fe304 and MnO, in good agreement with the related thermodynamic simulation. The obtained MnO was beneficial to stabilize the reduced MnFe2O4 and avoid serious sintering, although the oxygen in MnO was not fully utilized. Meanwhile, most sulfur present in LZ coal was converted to solid MnS during LZ reaction with MnFe2O4, which was further oxidized to MnSO4. Finally, the formation of both MnS and such manganese silicates as Mn2SiO4 and MnSiO3 should be addressed to ensure the full regeneration of the reduced MnFe2O4.
